@article{AnklamBehlerDingermannetal.2013, author = {Anklam, Elke and Behler, J{\"o}rg and Dingermann, Theodor and Elsinghorst, Paul and Fischer, Jochen and Esselen, Melanie and Foerster, Christian and Fr{\"o}hlich, Daniel and Goedel, Werner Andreas and Gregory, Peter and Grimme, Stefan and Hackenberger, Christian and Hansmann, Max and Heppekausen, Johannes and Hasenstab-Riedel, Sebastian and Kirchhoff, Erhard and Kratz, Karl-Ludwig and Krausz, Ferenc and Linker, Torsten and List, Benjamin and Ray, Kallol and Salzer, Reiner and Schubert, Ulrich and Schueth, Ferdi and Schwarz, Helmut and Schwietzke, Uta and Strey, Reinhard and Stumpf, Thorsten and Vaagt, Franziska and Volodkin, Dmitry and Wilke, Guenther and Zass, Engelbert and Zemb, Thomas}, title = {Awards}, series = {Nachrichten aus der Chemie : Zeitschrift der Gesellschaft Deutscher Chemiker}, volume = {61}, journal = {Nachrichten aus der Chemie : Zeitschrift der Gesellschaft Deutscher Chemiker}, number = {11}, publisher = {Ges. Dt. Chemiker}, address = {Frankfurt, Main}, issn = {1439-9598}, doi = {10.1002/nadc.201390372}, pages = {1145 -- 1148}, year = {2013}, language = {de} } @misc{SchottKretzschmarAckeretal.2014, author = {Schott, Juliane and Kretzschmar, Jerome and Acker, Margret and Eidner, Sascha and Kumke, Michael Uwe and Drobot, Bj{\"o}rn and Barkleit, Astrid and Taut, Steffen and Brendler, Vinzenz and Stumpf, Thorsten}, title = {Formation of a Eu(III) borate solid species from a weak Eu(III) borate complex in aqueous solution}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-98774}, pages = {13}, year = {2014}, abstract = {In the presence of polyborates (detected by 11B-NMR) the formation of a weak Eu(III) borate complex (lg β11 ∼ 2, estimated) was observed by time-resolved laser-induced fluorescence spectroscopy (TRLFS). This complex is a precursor for the formation of a solid Eu(III) borate species. The formation of this solid in solution was investigated by TRLFS as a function of the total boron concentration: the lower the total boron concentration, the slower is the solid formation. The solid Eu(III) borate was characterized by IR spectroscopy, powder XRD and solid-state TRLFS. The determination of the europium to boron ratio portends the existence of pentaborate units in the amorphous solid.}, language = {en} } @article{SchottKretzschmarAckeretal.2014, author = {Schott, Juliane and Kretzschmar, Jerome and Acker, Margret and Eidner, Sascha and Kumke, Michael Uwe and Drobot, Bjoern and Barkleit, Astrid and Taut, Steffen and Brendler, Vinzenz and Stumpf, Thorsten}, title = {Formation of a Eu(III) borate solid species from a weak Eu(III) borate complex in aqueous solution}, series = {Dalton transactions : a journal of inorganic chemistry, including bioinorganic, organometallic, and solid-state chemistry}, volume = {43}, journal = {Dalton transactions : a journal of inorganic chemistry, including bioinorganic, organometallic, and solid-state chemistry}, number = {30}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1477-9226}, doi = {10.1039/c4dt00843j}, pages = {11516 -- 11528}, year = {2014}, abstract = {In the presence of polyborates (detected by B-11-NMR) the formation of a weak Eu(III) borate complex (lg beta(11) similar to 2, estimated) was observed by time-resolved laser-induced fluorescence spectroscopy (TRLFS). This complex is a precursor for the formation of a solid Eu(III) borate species. The formation of this solid in solution was investigated by TRLFS as a function of the total boron concentration: the lower the total boron concentration, the slower is the solid formation. The solid Eu(III) borate was characterized by IR spectroscopy, powder XRD and solid-state TRLFS. The determination of the europium to boron ratio portends the existence of pentaborate units in the amorphous solid.}, language = {en} } @article{KretzschmarHaubitzHuebneretal.2018, author = {Kretzschmar, Jerome and Haubitz, Toni and Huebner, Rene and Weiss, Stephan and Husar, Richard and Brendler, Vinzenz and Stumpf, Thorsten}, title = {Network-like arrangement of mixed-valence uranium oxide nanoparticles after glutathione-induced reduction of uranium(VI)}, series = {Chemical communications}, volume = {54}, journal = {Chemical communications}, number = {63}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1359-7345}, doi = {10.1039/c8cc02070a}, pages = {8697 -- 8700}, year = {2018}, abstract = {Glutathione (GSH), a ubiquitous intracellular reducing tripeptide, is able to reduce hexavalent uranium, U(VI), to its tetravalent form, U(IV), in aqueous media in vitro, inducing the formation of nanocrystalline mixed-valence uranium oxide particles. After the initial reduction to U(V) and subsequent dismutation, the yielded U(IV) rapidly hydrolyses under near-neutral conditions forming 2-5 nm sized nanoparticles. The latter further aggregate to 20-40 nm chain-like building blocks that finally arrange as network-like structures.}, language = {en} } @article{HaubitzDrobotTsushimaetal.2021, author = {Haubitz, Toni and Drobot, Bj{\"o}rn and Tsushima, Satoru and Steudtner, Robin and Stumpf, Thorsten and Kumke, Michael Uwe}, title = {Quenching mechanism of uranyl(VI) by chloride and bromide in aqueous and non-aqueous solutions}, series = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory}, volume = {125}, journal = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory}, number = {20}, publisher = {American Chemical Society}, address = {Washington}, issn = {1089-5639}, doi = {10.1021/acs.jpca.1c02487}, pages = {4380 -- 4389}, year = {2021}, abstract = {A major hindrance in utilizing uranyl(VI) luminescence as a standard analytical tool, for example, in environmental monitoring or nuclear industries, is quenching by other ions such as halide ions, which are present in many relevant matrices of uranyl(VI) speciation. Here, we demonstrate through a combination of time-resolved laser-induced fluorescence spectroscopy, transient absorption spectroscopy, and quantum chemistry that coordinating solvent molecules play a crucial role in U(VI) halide luminescence quenching. We show that our previously suggested quenching mechanism based on an internal redox reaction of the 1:2-uranyl-halide-complex holds also true for bromide-induced quenching of uranyl(VI). By adopting specific organic solvents, we were able to suppress the separation of the oxidized halide ligand X-2(center dot-) and the formed uranyl(V) into fully solvated ions, thereby "reigniting" U(VI) luminescence. Time-dependent density functional theory calculations show that quenching occurs through the outer-sphere complex of U(VI) and halide in water, while the ligand-to-metal charge transfer is strongly reduced in acetonitrile.}, language = {en} } @article{HaubitzTsushimaSteudtneretal.2018, author = {Haubitz, Toni and Tsushima, Satoru and Steudtner, Robin and Drobot, Bj{\"o}rn and Geipel, Gerhard and Stumpf, Thorsten and Kumke, Michael Uwe}, title = {Ultrafast Transient Absorption Spectroscopy of UO(2)(2+)and [UO2Cl](+)}, series = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory}, volume = {122}, journal = {The journal of physical chemistry : A, Molecules, spectroscopy, kinetics, environment \& general theory}, number = {35}, publisher = {American Chemical Society}, address = {Washington}, issn = {1089-5639}, doi = {10.1021/acs.jpca.8b05567}, pages = {6970 -- 6977}, year = {2018}, abstract = {For the only water coordinated "free" uranyl (VI) aquo ion in perchlorate solution we identified and assigned several different excited states and showed that the (3)Delta state is the luminescent triplet state from transient absorption spectroscopy. With additional data from other spectroscopic methods (TRLFS, UV/vis) we generated a detailed Jablonski diagram and determined rate constants for several state transitions, like the inner conversion rate constant from the (3)Phi state to the (3)Delta state transition to be 0.35 ps(-1). In contrast to luminescence measurements, it was possible to observe the highly quenched uranyl(VI) ion in highly concentrated chloride solution by TAS and we were able to propose a dynamic quenching mechanism, where chloride complexation is followed by the charge transfer from the excited state uranyl(VI) to chloride. This proposed quenching route is supported by TD-DFT calculations.}, language = {en} }