Multidimensional spectroscopy uses sequences of optical pulses to study dynamical processes in complex molecules through correlation plots involving several time delay periods. Extensions of these techniques   to the x-ray regime will be discussed. Ultrafast nonlinear x-ray spectroscopy is made possible by newly developed free electron laser and high harmonic generation sources. The attosecond duration of X-ray pulses and the atomic selectivity of core X-ray excitations offer a uniquely high spatial and temporal resolution. We demonstrate how stimulated Raman detection of an X-ray probe may be used to monitor the phase and dynamics of the nonequilibrium valence electronic state wavepacket created by e.g. photoexcitation, photoionization and Auger processes.<br/><br/>Short X-ray pulses can directly detect the passage through conical intersections with the adequate temporal and spectral sensitivity. The technique is based on a coherent Raman process that employs a composite femtosecond/attosecond X-ray pulse to directly detect the electronic coherences (rather than populations) that are generated as the system passes through the conical intersections. X-ray pulses also offer a local probe of molecular chirality.<br/>

Ultrafast x-ray stimulated Raman spectroscopy and diffraction of molecules and molecular chirality

256th National Meeting (2018)

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.