Resolving Multiphoton Processes with High-Order Anisotropy Ultrafast X-ray Scattering

Abstract

We present first results on ultrafast X-ray scattering of strongly driven molecular Iodine and analysis of high-order anisotropic components of the scattering signal, up to four-photon absorption. We discuss the technical details of retrieving high fidelity high-order anisotropy components, and outline a method to analyze the scattering signal using Legendre decomposition. We use simulated anisotropic scattering signals and Fourier analysis to map how anisotropic dissociation motions can be extracted from the various Legendre orders. We observe multitude dissociation and vibration motions simultaneously arising from various multiphoton transitions. We use the anisotropy information of the scattering signal to disentangle the different processes and assign their dissociation velocities on the Angstrom and femtosecond scales de-novo.

20 pages, 6 figures

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Cited by in corpus (5)

• Real-Space Inversion and Super-Resolution of Ultrafast Scattering
• Ultrafast Molecular Frame Quantum Tomography
• A Laboratory Frame Density Matrix for Ultrafast Quantum Molecular Dynamics
• Applying Bayesian Inference and deterministic anisotropy to retrieve the molecular structure $|\Psi (\mathbf{R}){|}^2$ distribution from gas-phase diffraction experiments
• Optically induced anisotropy in time-resolved scattering: Imaging molecular scale structure and dynamics in disordered media with experiment and theory