Abstract
Recent advances in the generation of femtosecond extreme ultraviolet pulses have opened up the possibility to study final-state wave functions in photoemission experiments. Here, we investigate, for the first time using femtosecond time-resolved core-level spectroscopy, the feasibility of observing the buildup of a state correlation in a direct time domain. Giant changes in the ratio of photoemission cross-sections of spin-orbit split core states, the branching ratio, are identified. Multi-configuration Dirac-Fock calculations show that the origin of the branching ratio deviation is due to strong core-valence interactions. The possibility to tune this interaction by charge transfer offers intriguing opportunities to study correlation effects in solid and molecular systems in the future.
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