TY  - JOUR
A1  - Schreck, Simon
A1  - Pietzsch, Annette
A1  - Kennedy, Brian
A1  - Sathe, Conny
A1  - Miedema, Piter S.
A1  - Techert, Simone
A1  - Strocov, Vladimir N.
A1  - Schmitt, Thorsten
A1  - Hennies, Franz
A1  - Rubensson, Jan-Erik
A1  - Föhlisch, Alexander
T1  - Ground state potential energy surfaces around selected atoms from resonant inelastic x-ray scattering
JF  - Scientific reports
N2  - Thermally driven chemistry as well as materials’ functionality are determined by the potential energy surface of a systems electronic ground state. This makes the potential energy surface a central and powerful concept in physics, chemistry and materials science. However, direct experimental access to the potential energy surface locally around atomic centers and to its long-range structure are lacking. Here we demonstrate how sub-natural linewidth resonant inelastic soft x-ray scattering at vibrational resolution is utilized to determine ground state potential energy surfaces locally and detect long-range changes of the potentials that are driven by local modifications. We show how the general concept is applicable not only to small isolated molecules such as O2 but also to strongly interacting systems such as the hydrogen bond network in liquid water. The weak perturbation to the potential energy surface through hydrogen bonding is observed as a trend towards softening of the ground state potential around the coordinating atom. The instrumental developments in high resolution resonant inelastic soft x-ray scattering are currently accelerating and will enable broad application of the presented approach. With this multidimensional potential energy surfaces that characterize collective phenomena such as (bio)molecular function or high-temperature superconductivity will become accessible in near future.
Y1  - 2016
U6  - https://doi.org/10.1038/srep20054
SN  - 2045-2322
VL  - 6
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Kunnus, Kristjan
A1  - Josefsson, Ida
A1  - Rajkovic, Ivan
A1  - Schreck, Simon
A1  - Quevedo, Wilson
A1  - Beye, Martin
A1  - Grübel, Sebastian
A1  - Scholz, Mirko
A1  - Nordlund, Dennis
A1  - Zhang, Wenkai
A1  - Hartsock, Robert W.
A1  - Gaffney, Kelly J.
A1  - Schlotter, William F.
A1  - Turner, Joshua J.
A1  - Kennedy, Brian
A1  - Hennies, Franz
A1  - Techert, Simone
A1  - Wernet, Philippe
A1  - Odelius, Michael
A1  - Föhlisch, Alexander
T1  - Anti-Stokes resonant x-ray Raman scattering for atom specific and excited state selective dynamics
JF  - NEW JOURNAL OF PHYSICS
N2  - 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.
KW  - ultrafast photochemistry
KW  - excited state selectivity
KW  - anti-Stokes resonant x-ray raman scattering
KW  - free electron lasers
KW  - resonant inelastic x-ray scattering
Y1  - 2016
U6  - https://doi.org/10.1088/1367-2630/18/10/103011
SN  - 1367-2630
VL  - 18
PB  - IOP Publ. Ltd.
CY  - Bristol
ER  -