Resonantly-Enhanced Difference-Frequency Generation in the Core X-ray Absorption of Molecules
2021
We use real-time time-dependent density functional theory simulations to numerically demonstrate that
resonantly-enhanced difference-frequency generation (re-DFG)
involving intense ultrashort coherent X-ray pulses can selectively excite core states of atoms in molecules.
As a model case, we evaluate the spectral selectivity of re-DFG excitation of the oxygen K-edge
by illumination of a single gas-phase water molecule with two-color X-ray
pulses of different photon energies and durations.
The re-DFG excitation is further probed by a small delayed pulse
with central photon energy resonant with the oxygen K-edge peak absorption line.
Based on these results, we anticipate that highly selective excitation by re-DFG
X-ray nonlinear processes might be achieved in more complex molecular systems and bulk materials by
using highly penetrating two-color hard X-ray pulses, with extensive applications.
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