X-ray transient absorption spectroscopy by an ultrashort x-ray-laser pulse in a continuous-wave IR field

Abstract

X-ray transient absorption spectra (XTAS) of molecules are theoretically investigated in a femtosecond x-ray pump and continuous-wave (cw) infrared (IR)-control scenario. The scheme is exemplified by a CO pulse, while dynamic Stark shifts are induced by the cw IR-control radiation. As a result, significant shoulder molecule resonantly pumped into carbon and oxygen core-excited 1s → π∗ states by a weak femtosecond x-ray structures appear in XTAS showing strong dependence on the phase of IR radiation relative to the envelope of the x-ray pulse. Due to a significant difference in the frequencies of the two pulses, the present XTAS scheme provides much clear interpretation of the dynamic Stark effects as compared to the attosecond UV transient absorption scenario. Within the suggested two-level model, where the total spectrum is decomposed as incoherent superposition of contributions from different vibrational excitations weighted by the Franck-Condon Factors, all spectral structures can be well identified and interpreted in a good agreement with the full-scale molecular simulations.Well-characterized XTAS in the proposed IR-control scheme can be applied for fine phase synchronization between IR and x-ray pulses, highly demanded in modern experiments on x-ray free-electron lasers.