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Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
(2022)
Mayer, Dennis ; Lever, Fabiano ; Picconi, David ; Metje, Jan ; Ališauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Ehlert, Christopher ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard James ; Trabattoni, Andrea ; Wallner, Måns ; Saalfrank, Peter ; Wolf, Thomas J. A. ; Gühr, Markus
The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy
(2022)
Mayer, Dennis ; Lever, Fabiano ; Picconi, David ; Metje, Jan ; Ališauskas, Skirmantas ; Calegari, Francesca ; Düsterer, Stefan ; Ehlert, Christopher ; Feifel, Raimund ; Niebuhr, Mario ; Manschwetus, Bastian ; Kuhlmann, Marion ; Mazza, Tommaso ; Robinson, Matthew Scott ; Squibb, Richard James ; Trabattoni, Andrea ; Wallner, Måns ; Saalfrank, Peter ; Wolf, Thomas J. A. ; Gühr, Markus
The conversion of photon energy into other energetic forms in molecules is accompanied by charge moving on ultrafast timescales. We directly observe the charge motion at a specific site in an electronically excited molecule using time-resolved x-ray photoelectron spectroscopy (TR-XPS). We extend the concept of static chemical shift from conventional XPS by the excited-state chemical shift (ESCS), which is connected to the charge in the framework of a potential model. This allows us to invert TR-XPS spectra to the dynamic charge at a specific atom. We demonstrate the power of TR-XPS by using sulphur 2p-core-electron-emission probing to study the UV-excited dynamics of 2-thiouracil. The method allows us to discover that a major part of the population relaxes to the molecular ground state within 220–250 fs. In addition, a 250-fs oscillation, visible in the kinetic energy of the TR-XPS, reveals a coherent exchange of population among electronic states.
Kalinkat, Gregor ; Cabral, Juliano Sarmento ; Darwall, William ; Ficetola, G. Francesco ; Fisher, Judith L. ; Giling, Darren P. ; Gosselin, Marie-Pierre ; Grossart, Hans-Peter ; Jaehnig, Sonja C. ; Jeschke, Jonathan M. ; Knopf, Klaus ; Larsen, Stefano ; Onandia, Gabriela ; Paetzig, Marlene ; Saul, Wolf-Christian ; Singer, Gabriel ; Sperfeld, Erik ; Jaric, Ivan
Heger, Tina ; Bernard-Verdier, Maud ; Gessler, Arthur ; Greenwood, Alex D. ; Grossart, Hans-Peter ; Hilker, Monika ; Keinath, Silvia ; Kowarik, Ingo ; Küffer, Christoph ; Marquard, Elisabeth ; Mueller, Johannes ; Niemeier, Stephanie ; Onandia, Gabriela ; Petermann, Jana S. ; Rillig, Matthias C. ; Rodel, Mark-Oliver ; Saul, Wolf-Christian ; Schittko, Conrad ; Tockner, Klement ; Joshi, Jasmin Radha ; Jeschke, Jonathan M.
Global change has complex eco-evolutionary consequences for organisms and ecosystems, but related concepts (e.g., novel ecosystems) do not cover their full range. Here we propose an umbrella concept of "ecological novelty" comprising (1) a site-specific and (2) an organism-centered, eco-evolutionary perspective. Under this umbrella, complementary options for studying and communicating effects of global change on organisms, ecosystems, and landscapes can be included in a toolbox. This allows researchers to address ecological novelty from different perspectives, e.g., by defining it based on (a) categorical or continuous measures, (b) reference conditions related to sites or organisms, and (c) types of human activities. We suggest striving for a descriptive, non-normative usage of the term "ecological novelty" in science. Normative evaluations and decisions about conservation policies or management are important, but require additional societal processes and engagement with multiple stakeholders.