Theory of ultrafast x-ray scattering by molecules in the gas phase

We recast existing theory of ultrafast time-resolved x-ray scattering by molecules in the gas phase into a unified and coherent framework based on first-order time-dependent perturbation theory and quantum electrodynamics. The effect of the detection window is analyzed in detail and the contributions to the total scattering signal are discussed. This includes the coherent mixed component caused by interference between scattering amplitudes from different electronic states. A new, detailed, and fully converged simulation of ultrafast total x-ray scattering by excited H-2 molecules illustrates the theory and demonstrates that the inelastic component can contribute strongly to the total difference scattering signal, i.e., on the same order of magnitude as the elastic component.