Recent ultrabright sources of x-ray radiation will enable nonlinear excitation at x-ray frequencies, allowing molecular valence electron dynamics to be directly observed. Pump-probe, stimulated Raman, and photon echo experiments developed to probe vibrational and optical excitonic systems are adapted to describe the valence reponse to multiple core-excitations. New expressions including rotational averaging and effective core-valence interactions with reduced computational cost are proposed. The time-resolved photoemission spectra provides another measurement channel for observing electronic dynamics. Translating these new high energy time- and frequency-domain techniques to nonlinear experiments represents a substantial theoretical challenge.
|Commitee:||Mandelshtam, Vladimir A., Martens, Craig|
|School:||University of California, Irvine|
|Department:||Chemistry - Ph.D.|
|School Location:||United States -- California|
|Source:||DAI-B 73/05, Dissertation Abstracts International|
|Subjects:||Physical chemistry, Molecular physics, Theoretical physics|
|Keywords:||Electron dynamics, Nonlinear spectroscopy, Nonlinear x-ray spectroscopy, Resonant inelastic x-ray spectroscopy, Time-resolved photoemission, Ultrashort time, X-ray absorption near-edge structure|
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