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

• 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.

Ämnesord

NATURVETENSKAP  -- Fysik (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences (hsv//eng)

NATURVETENSKAP  -- Fysik -- Acceleratorfysik och instrumentering (hsv//swe)

NATURAL SCIENCES  -- Physical Sciences -- Accelerator Physics and Instrumentation (hsv//eng)

Nyckelord

ultrafast photochemistry

excited state selectivity

anti-Stokes resonant x-ray raman scattering

free electron lasers

resonant inelastic x-ray scattering

anti-Stokes resonant x-ray raman scattering

excited state selectivity

free electron lasers

resonant inelastic x-ray scattering

ultrafast photochemistry

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