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Effects of Electronic Coherence in Ultrafast Spectroscopy

Abstract

Electronic dynamics takes place at the attosecond timescale. Recent technological advancements permit the creation of light pulses with durations in the attosecond regime, opening up the possibility of monitoring this ultrafast dynamics in real time. In particular, it becomes possible to observe the time-dependent interference between material electronic states, thus tracking the electronic energies temporally. This information, originating in the coherence terms in the electronic density matrix, can provide spectral information in the time-domain. Such an approach is particularly useful when the desired information is transient. In this thesis, we examine how electronic coherences contribute to photoelectron and a variety of x-ray Raman signals. We then utilize photoelectron spectroscopy and linear off-resonant Raman (TRUECARS) to track the dynamics of a model system by way of example.

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