TY  - JOUR
A1  - Kretzschmar, Jerome
A1  - Haubitz, Toni
A1  - Huebner, Rene
A1  - Weiss, Stephan
A1  - Husar, Richard
A1  - Brendler, Vinzenz
A1  - Stumpf, Thorsten
T1  - Network-like arrangement of mixed-valence uranium oxide nanoparticles after glutathione-induced reduction of uranium(VI)
JF  - Chemical communications
N2  - 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.
Y1  - 2018
U6  - https://doi.org/10.1039/c8cc02070a
SN  - 1359-7345
SN  - 1364-548X
VL  - 54
IS  - 63
SP  - 8697
EP  - 8700
PB  - Royal Society of Chemistry
CY  - Cambridge
ER  - 
TY  - JOUR
A1  - Oertel, Jana
A1  - Keller, Adrian
A1  - Prinz, Julia
A1  - Schreiber, Benjamin
A1  - Huebner, Rene
A1  - Kerbusch, Jochen
A1  - Bald, Ilko
A1  - Fahmy, Karim
T1  - Anisotropic metal growth on phospholipid nanodiscs via lipid bilayer expansion
JF  - Scientific reports
N2  - Self-assembling biomolecules provide attractive templates for the preparation of metallic nanostructures. However, the intuitive transfer of the "outer shape" of the assembled macromolecules to the final metallic particle depends on the intermolecular forces among the biomolecules which compete with interactions between template molecules and the metal during metallization. The shape of the bio-template may thus be more dynamic than generally assumed. Here, we have studied the metallization of phospholipid nanodiscs which are discoidal particles of similar to 10 nm diameter containing a lipid bilayer similar to 5 nm thick. Using negatively charged lipids, electrostatic adsorption of amine-coated Au nanoparticles was achieved and followed by electroless gold deposition. Whereas Au nanoparticle adsorption preserves the shape of the bio-template, metallization proceeds via invasion of Au into the hydrophobic core of the nanodisc. Thereby, the lipidic phase induces a lateral growth that increases the diameter but not the original thickness of the template. Infrared spectroscopy reveals lipid expansion and suggests the existence of internal gaps in the metallized nanodiscs, which is confirmed by surface-enhanced Raman scattering from the encapsulated lipids. Interference of metallic growth with non-covalent interactions can thus become itself a shape-determining factor in the metallization of particularly soft and structurally anisotropic biomaterials.
Y1  - 2016
U6  - https://doi.org/10.1038/srep26718
SN  - 2045-2322
VL  - 6
PB  - Nature Publ. Group
CY  - London
ER  - 
TY  - JOUR
A1  - Shivhare, Rishi
A1  - Erdmann, Tim
A1  - Hoermann, Ulrich
A1  - Collado-Fregoso, Elisa
A1  - Zeiske, Stefan
A1  - Benduhn, Johannes
A1  - Ullbrich, Sascha
A1  - Huebner, Rene
A1  - Hambsch, Mike
A1  - Kiriy, Anton
A1  - Voit, Brigitte
A1  - Neher, Dieter
A1  - Vandewal, Koen
A1  - Mannsfeld, Stefan C. B.
T1  - Alkyl Branching Position in Diketopyrrolopyrrole Polymers
BT  - Interplay between Fibrillar Morphology and Crystallinity and Their Effect on Photogeneration and Recombination in Bulk-Heterojunction Solar Cells
JF  - Chemistry of materials : a publication of the American Chemical Society
N2  - Diketopyrrolopyrrole (DPP)-based donor acceptor copolymers have gained a significant amount of research interest in the organic electronics community because of their high charge carrier mobilities in organic field-effect transistors (OFETs) and their ability to harvest near-infrared (NIR) photons in solar cells. In this study, we have synthesized four DPP based donor-acceptor copolymers with variations in the donor unit and the branching point of the solubilizing alkyl chains (at the second or sixth carbon position). Grazing incidence wide-angle X-ray scattering (GIWAXS) results suggest that moving the branching point further away from the polymer backbone increases the tendency for aggregation and yields polymer phases with a higher degree of crystallinity (DoC). The polymers were blended with PC70BM and used as active layers in solar cells. A careful analysis of the energetics of the neat polymer and blend films reveals that the charge-transfer state energy (E-CT) of the blend films lies exceptionally close to the singlet energy of the donor (E-D*), indicating near zero electron transfer losses. The difference between the optical gap and open-circuit voltage (V-OC) is therefore determined to be due to rather high nonradiative 418 +/- 13 mV) and unavoidable radiative voltage losses (approximate to 255 +/- 8 mV). Even though the four materials have similar optical gaps, the short-circuit current density (J(SC)) covers a vast span from 7 to 18 mA cm(-2) for the best performing system. Using photoluminescence (PL) quenching and transient charge extraction techniques, we quantify geminate and nongeminate losses and find that fewer excitons reach the donor-acceptor interface in polymers with further away branching points due to larger aggregate sizes. In these material systems, the photogeneration is therefore mainly limited by exciton harvesting efficiency.
Y1  - 2018
U6  - https://doi.org/10.1021/acs.chemmater.8b02739
SN  - 0897-4756
SN  - 1520-5002
VL  - 30
IS  - 19
SP  - 6801
EP  - 6809
PB  - American Chemical Society
CY  - Washington
ER  -