Abstract
X-ray absorption and core-ionization spectra of molecules pumped by two coherent infrared pulses with different polarizations are studied theoretically. We have found a sensitivity of the vibrational profile of x-ray probe spectra to polarizations of the IR and x-ray pulses. This polarization dependence is qualitatively different for x-ray absorption and x-ray photoelectron spectra. Measurements of this polarization dependence allow to select the difference in Franck-Condon distributions from the lowest and pumped vibrational levels of the electronic ground state. The proposed technique is exemplified numerically using x-ray absorption spectra of the pumped CO molecule. We also show that this kind of pump-probe spectroscopy can enable studies of the dynamics of molecular rotation.
Highlights
Interactions of intense electromagnetic pulses with matter are attracting increasing interest due to its intrinsic potential to investigate the dynamics of quantum systems in real timescales and because of the possibility to manipulate quantum states
The proposed technique is exemplified numerically using x-ray absorption spectra of the pumped CO molecule. We show that this kind of pump-probe spectroscopy can enable studies of the dynamics of molecular rotation
As the probe we study the possibility of using x-ray absorption and x-ray photoelectron spectroscopy
Summary
Interactions of intense electromagnetic pulses with matter are attracting increasing interest due to its intrinsic potential to investigate the dynamics of quantum systems in real timescales and because of the possibility to manipulate quantum states. The use of polarization sensitive techniques is common in many time-resolved optical pump-probe experiments [4]. In this context, resonant inelastic x-ray scattering (RIXS) can be considered as a special kind of pump-probe spectroscopy. We explore the polarization sensitivity of x-ray absorption and x-ray photoionization of molecules pumped by two coherent, time-delayed, and linearly polarized long IR pulses. The main reason for the polarization sensitivity of IR + x-ray pump-probe absorption spectra is the different orientation of the transition dipoles moments of the IR transition and the electronic transition of core excitation.
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