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DOE OSTI · 1887211

Optically Induced Anisotropy in Time-Resolved Scattering: Imaging Molecular-Scale Structure and Dynamics in Disordered Media with Experiment and Theory

Montoya-Castillo, Andrés·Chen, Michael S.·Raj, Sumana L.·Jung, Kenneth A.·Kjaer, Kasper S.·Morawietz, Tobias·Gaffney, Kelly J.·van Driel, Tim B.·Markland, Thomas E.
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Abstract

Time-resolved scattering experiments enable imaging of materials at the molecular scale with femtosecond time resolution. However, in disordered media they provide access to just one radial dimension thus limiting the study of orientational structure and dynamics. Here we introduce a rigorous and practical theoretical framework for predicting and interpreting experiments combining optically induced anisotropy and time-resolved scattering. Using impulsive nuclear Raman and ultrafast x-ray scattering experiments of chloroform and simulations, we demonstrate that this framework can accurately predict and elucidate both the spatial and temporal features of these experiments.

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75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITYKerr effectRaman spectroscopyequilibrium fluctuationsfour-wave mixinglinear response theorymolecular dynamicsnonequilibrium fluctuationsnonlinear opticspump-probe spectroscopyquantum formalismquantum statistical mechanicssymmetries in condensed mattertime resolved light scattering spectroscopyx-ray scattering

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Montoya-Castillo, Andrés, Chen, Michael S., Raj, Sumana L., Jung, Kenneth A., Kjaer, Kasper S., Morawietz, Tobias, Gaffney, Kelly J., van Driel, Tim B., Markland, Thomas E.. 2022-07-29. Optically Induced Anisotropy in Time-Resolved Scattering: Imaging Molecular-Scale Structure and Dynamics in Disordered Media with Experiment and Theory. https://doi.org/10.1103/physrevlett.129.056001

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