Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics

oleh: Kristjan Kunnus, Ida Josefsson, Ivan Rajkovic, Simon Schreck, Wilson Quevedo, Martin Beye, Sebastian Grübel, Mirko Scholz, Dennis Nordlund, Wenkai Zhang, Robert W Hartsock, Kelly J Gaffney, William F Schlotter, Joshua J Turner, Brian Kennedy, Franz Hennies, Simone Techert, Philippe Wernet, Michael Odelius, Alexander Föhlisch

Format: Article
Diterbitkan: IOP Publishing 2016-01-01

Deskripsi

Ultrafast electronic and structural dynamics of matter govern rate and selectivity of chemical reactions, as well as phase transitions and efficient switching in functional materials. Since x-rays determine electronic and structural properties with elemental, chemical, orbital and magnetic selectivity, short pulse x-ray sources have become central enablers of ultrafast science. Despite of these strengths, ultrafast x-rays have been poor at picking up excited state moieties from the unexcited ones. With time-resolved anti-Stokes resonant x-ray Raman scattering (AS-RXRS) performed at the LCLS, and ab initio theory we establish background free excited state selectivity in addition to the elemental, chemical, orbital and magnetic selectivity of x-rays. This unparalleled selectivity extracts low concentration excited state species along the pathway of photo induced ligand exchange of Fe(CO) _5 in ethanol. Conceptually a full theoretical treatment of all accessible insights to excited state dynamics with AS-RXRS with transform-limited x-ray pulses is given—which will be covered experimentally by upcoming transform-limited x-ray sources.