@phdthesis{Friess2016, author = {Frieß, Fabian}, title = {Shape-memory polymer micronetworks}, school = {Universit{\"a}t Potsdam}, pages = {xiv, 111 S.}, year = {2016}, language = {en} } @article{GallandiMaromRinkeetal.2016, author = {Gallandi, Lukas and Marom, Noa and Rinke, Patrick and K{\"o}rzd{\"o}rfer, Thomas}, title = {Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules II: Non-Empirically Tuned Long-Range Corrected Hybrid Functionals}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.5b00873}, pages = {605 -- 614}, year = {2016}, abstract = {The performance of non-empirically tuned long-range corrected hybrid functionals for the prediction of vertical ionization potentials (IPs) and electron affinities (EAs) is assessed for a set of 24 organic acceptor molecules. Basis set extrapolated coupled cluster singles, doubles, and perturbative triples [CCSD(T)] calculations serve as a reference for this study. Compared to standard exchange-correlation functionals, tuned long-range corrected hybrid functionals produce highly reliable results for vertical IPs and EAs, yielding mean absolute errors on par with computationally more demanding GW calculations. In particular, it is demonstrated that long-range corrected hybrid functionals serve as ideal starting points for non-self-consistent GW calculations.}, language = {en} } @misc{GangloffUlbrichtLorsonetal.2016, author = {Gangloff, Niklas and Ulbricht, Juliane and Lorson, Thomas and Schlaad, Helmut and Luxenhofer, Robert}, title = {Peptoids and Polypeptoids at the Frontier of Supra- and Macromolecular Engineering}, series = {Chemical reviews}, volume = {116}, journal = {Chemical reviews}, publisher = {American Chemical Society}, address = {Washington}, issn = {0009-2665}, doi = {10.1021/acs.chemrev.5b00201}, pages = {1753 -- 1802}, year = {2016}, language = {en} } @article{GuietUnmuessigGoebeletal.2016, author = {Guiet, Amandine and Unm{\"u}ssig, Tobias and G{\"o}bel, Caren and Vainio, Ulla and Wollgarten, Markus and Driess, Matthias and Schlaad, Helmut and Polte, J{\"o}rg and Fischer, Anna}, title = {Yolk@Shell Nanoarchitectures with Bimetallic Nanocores - Synthesis and Electrocatalytic Applications}, series = {Earth \& planetary science letters}, volume = {8}, journal = {Earth \& planetary science letters}, publisher = {American Chemical Society}, address = {Washington}, issn = {1944-8244}, doi = {10.1021/acsami.6b06595}, pages = {28019 -- 28029}, year = {2016}, language = {en} } @article{GoebelStoltenbergKrehletal.2016, author = {G{\"o}bel, Ronald and Stoltenberg, Marcus and Krehl, Stefan and Biolley, Christine and Rothe, Regina and Schmidt, Bernd and Hesemann, Peter and Taubert, Andreas}, title = {A Modular Approach towards Mesoporous Silica Monoliths with Organically Modified Pore Walls: Nucleophilic Addition, Olefin Metathesis, and Cycloaddition}, series = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, volume = {6}, journal = {European journal of inorganic chemistry : a journal of ChemPubSoc Europe}, publisher = {Wiley-VCH}, address = {Weinheim}, issn = {1434-1948}, doi = {10.1002/ejic.201500638}, pages = {2088 -- 2099}, year = {2016}, abstract = {We have synthesized mesoporous silica (monoliths) with defined surface chemistry by means of a number of addition reactions: (i) coupling of an isocyanate to a surface-immobilized thiol, (ii) addition of an epoxide to a surface-immobilized thiol, (iii) cross-metathesis between two olefins, and (iv) Huisgen [2+3] cycloaddition of an alkyne-functionalized silica monolith with an azide. Functionalization of the mesopores was observed, but there are significant differences between individual approaches. Isocyanate and epoxide additions lead to high degrees of functionalization, whereas olefin metathesis and [2+3] cycloaddition are less effective. We further show that the efficiency of the modification is about twice as high in mesoporous silica particles than in macroscopic silica monoliths.}, language = {en} } @article{HardyTorresRendonLealEganaetal.2016, author = {Hardy, John G. and Torres-Rendon, Jose Guillermo and Leal-Egana, Aldo and Walther, Andreas and Schlaad, Helmut and Coelfen, Helmut and Scheibel, Thomas R.}, title = {Biomineralization of Engineered Spider Silk Protein-Based Composite Materials for Bone Tissue Engineering}, series = {Materials}, volume = {9}, journal = {Materials}, publisher = {MDPI}, address = {Basel}, issn = {1996-1944}, doi = {10.3390/ma9070560}, pages = {93 -- 108}, year = {2016}, abstract = {Materials based on biodegradable polyesters, such as poly(butylene terephthalate) (PBT) or poly(butylene terephthalate-co-poly(alkylene glycol) terephthalate) (PBTAT), have potential application as pro-regenerative scaffolds for bone tissue engineering. Herein, the preparation of films composed of PBT or PBTAT and an engineered spider silk protein, (eADF4(C16)), that displays multiple carboxylic acid moieties capable of binding calcium ions and facilitating their biomineralization with calcium carbonate or calcium phosphate is reported. Human mesenchymal stem cells cultured on films mineralized with calcium phosphate show enhanced levels of alkaline phosphatase activity suggesting that such composites have potential use for bone tissue engineering.}, language = {en} } @article{HerfurthLaschewskyNoirezetal.2016, author = {Herfurth, Christoph and Laschewsky, Andre and Noirez, Laurence and von Lospichl, Benjamin and Gradzielski, Michael}, title = {Thermoresponsive (star) block copolymers from one-pot sequential RAFT polymerizations and their self-assembly in aqueous solution}, series = {Polymer : the international journal for the science and technology of polymers}, volume = {107}, journal = {Polymer : the international journal for the science and technology of polymers}, publisher = {Elsevier}, address = {Oxford}, issn = {0032-3861}, doi = {10.1016/j.polymer.2016.09.089}, pages = {422 -- 433}, year = {2016}, abstract = {A series of hydrophobically end-capped linear triblock copolymers as well as of three-arm and four-arm star block copolymers was synthesized in a one-pot procedure from N,N-dimethylacrylamide (DMA) and N, N-diethylacrylamide (DEA). The sequential reversible addition-fragmentation chain transfer (RAFT) polymerization of these monomers via the R-approach using bi-, tri- and tetrafunctional chain transfer agents (CrAs) bearing hydrophobic dodecyl moieties proceeded in a well-controlled manner up to almost quantitative conversion. Polymers with molar masses up to 150 kDa, narrow molar mass distribution (PDI <= 1.3) and high end group functionality were obtained, which are thermoresponsive in aqueous solution showing a LCST (lower critical solution temperature) transition. The temperature-dependent associative behavior of the polymers was examined using turbidimetry, static and dynamic light scattering (SLS, DLS), and small angle neutron scattering (SANS) for structural analysis. At 25 degrees C, the polymers form weak transient networks, and rather small hydrophobic domains are already present for polymer concentrations of 5 wt\%. However, when heating above the LCST transition (35-40 degrees C) of the PDEA blocks, the enhanced formation of hydrophobic domains is observed by means of light and neutron scattering. These domains have a size of about 12-15 nm and must be effectively physically cross-linked as they induce high viscosity for the more concentrated samples. SANS shows that these domains are ordered as evidenced by the appearance of a correlation peak. The copolymer architecture affects in particular the extent of ordering as the four-arm star block copolymer shows much more repulsive interactions compared to the analogous copolymers with a lower number of arms. (C) 2016 Elsevier Ltd. All rights reserved.}, language = {en} } @phdthesis{Hildebrand2016, author = {Hildebrand, Viet}, title = {Twofold switchable block copolymers based on new polyzwitterions}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-101372}, school = {Universit{\"a}t Potsdam}, pages = {xvi, 170, LXXX}, year = {2016}, abstract = {In complement to the well-established zwitterionic monomers 3-((2-(methacryloyloxy)ethyl)dimethylammonio)propane-1-sulfonate ("SPE") and 3-((3-methacrylamidopropyl)dimethylammonio)propane-1-sulfonate ("SPP"), the closely related sulfobetaine monomers were synthesized and polymerized by reversible addition-fragmentation chain transfer (RAFT) polymerization, using a fluorophore labeled RAFT agent. The polyzwitterions of systematically varied molar mass were characterized with respect to their solubility in water, deuterated water, and aqueous salt solutions. These poly(sulfobetaine)s show thermoresponsive behavior in water, exhibiting upper critical solution temperatures (UCST). Phase transition temperatures depend notably on the molar mass and polymer concentration, and are much higher in D2O than in H2O. Also, the phase transition temperatures are effectively modulated by the addition of salts. The individual effects can be in parts correlated to the Hofmeister series for the anions studied. Still, they depend in a complex way on the concentration and the nature of the added electrolytes, on the one hand, and on the detailed structure of the zwitterionic side chain, on the other hand. For the polymers with the same zwitterionic side chain, it is found that methacrylamide-based poly(sulfobetaine)s exhibit higher UCST-type transition temperatures than their methacrylate analogs. The extension of the distance between polymerizable unit and zwitterionic groups from 2 to 3 methylene units decreases the UCST-type transition temperatures. Poly(sulfobetaine)s derived from aliphatic esters show higher UCST-type transition temperatures than their analogs featuring cyclic ammonium cations. The UCST-type transition temperatures increase markedly with spacer length separating the cationic and anionic moieties from 3 to 4 methylene units. Thus, apparently small variations of their chemical structure strongly affect the phase behavior of the polyzwitterions in specific aqueous environments. Water-soluble block copolymers were prepared from the zwitterionic monomers and the non-ionic monomer N-isopropylmethacrylamide ("NIPMAM") by the RAFT polymerization. Such block copolymers with two hydrophilic blocks exhibit twofold thermoresponsive behavior in water. The poly(sulfobetaine) block shows an UCST, whereas the poly(NIPMAM) block exhibits a lower critical solution temperature (LCST). This constellation induces a structure inversion of the solvophobic aggregate, called "schizophrenic micelle". Depending on the relative positions of the two different phase transitions, the block copolymer passes through a molecularly dissolved or an insoluble intermediate regime, which can be modulated by the polymer concentration or by the addition of salt. Whereas, at low temperature, the poly(sulfobetaine) block forms polar aggregates that are kept in solution by the poly(NIPMAM) block, at high temperature, the poly(NIPMAM) block forms hydrophobic aggregates that are kept in solution by the poly(sulfobetaine) block. Thus, aggregates can be prepared in water, which switch reversibly their "inside" to the "outside", and vice versa.}, language = {en} } @article{HildebrandLaschewskyWischerhoff2016, author = {Hildebrand, Viet and Laschewsky, Andre and Wischerhoff, Erik}, title = {Modulating the solubility of zwitterionic poly((3methacrylamidopropyl)ammonioalkane sulfonate)s in water and aqueous salt solutions via the spacer group separating the cationic and the anionic moieties}, series = {Polymer Chemistry}, volume = {7}, journal = {Polymer Chemistry}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1759-9954}, doi = {10.1039/c5py01642h}, pages = {731 -- 740}, year = {2016}, abstract = {Complementary to the well-established zwitterionic monomer 3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SPP), the closely related monomers 2-hydroxy-3-((3-methacrylamidopropyl) dimethylammonio) propane-1-sulfonate (SHPP) and 4-((3-methacrylamidopropyl) dimethylammonio)butane- 1-sulfonate (SBP) were synthesised and polymerised by reversible addition-fragmentation chain transfer (RAFT) polymerisation, using a fluorophore labeled RAFT agent. The polyzwitterions of systematically varied molar masses were characterised with respect to their solubility in water and aqueous salt solutions. Both poly(sulfobetaine)s show thermoresponsive behaviour in water, exhibiting phase separation at low temperatures and upper critical solution temperatures (UCST). For both polySHPP and polySBP, cloud points depend notably on the molar mass, and are much higher in D2O than in H2O. Also, the cloud points are effectively modulated by the addition of salts. The individual effects can be in parts correlated to the Hofmeister series for the anions studied. Still, they depend in a complex way on the concentration and the nature of the added electrolytes, on the one hand, and on the detailed nature of the spacer group separating the anionic and the cationic charges of the betaine moiety, on the other hand. As anticipated, the cloud points of polySBP are much higher than the ones of the analogous polySPP of identical molar mass. Surprisingly, the cloud points of polySHPP are also somewhat higher than the ones of their polySPP analogues, despite the additional hydrophilic hydroxyl group present in the spacer separating the ammonium and the sulfonate moieties. These findings point to a complicated interplay of the various hydrophilic components in polyzwitterions with respect to their overall hydrophilicity. Thus, the spacer group in the betaine moiety proves to be an effective additional molecular design parameter, apparently small variations of which strongly influence the phase behaviour of the polyzwitterions in specific aqueous environments.}, language = {en} } @misc{HildebrandLaschewskyPaechetal.2016, author = {Hildebrand, Viet and Laschewsky, Andr{\´e} and P{\"a}ch, Michael and M{\"u}ller-Buschbaum, Peter and Papadakis, Christine M.}, title = {Effect of the zwitterion structure on the thermo-responsive behaviour of poly(sulfobetaine methacrylates)}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-102028}, pages = {13}, year = {2016}, abstract = {A series of new sulfobetaine methacrylates, including nitrogen-containing saturated heterocycles, was synthesised by systematically varying the substituents of the zwitterionic group. Radical polymerisation via the RAFT (reversible addition-fragmentation chain transfer) method in trifluoroethanol proceeded smoothly and was well controlled, yielding polymers with predictable molar masses. Molar mass analysis and control of the end-group fidelity were facilitated by end-group labeling with a fluorescent dye. The polymers showed distinct thermo-responsive behaviour of the UCST (upper critical solution temperature) type in an aqueous solution, which could not be simply correlated to their molecular structure via an incremental analysis of the hydrophilic and hydrophobic elements incorporated within them. Increasing the spacer length separating the ammonium and the sulfonate groups of the zwitterion moiety from three to four carbons increased the phase transition temperatures markedly, whereas increasing the length of the spacer separating the ammonium group and the carboxylate ester group on the backbone from two to three carbons provoked the opposite effect. Moreover, the phase transition temperatures of the analogous polyzwitterions decreased in the order dimethylammonio > morpholinio > piperidinio alkanesulfonates. In addition to the basic effect of the polymers' precise molecular structure, the concentration and the molar mass dependence of the phase transition temperatures were studied. Furthermore, we investigated the influence of added low molar mass salts on the aqueous-phase behaviour for sodium chloride and sodium bromide as well as sodium and ammonium sulfate. The strong effects evolved in a complex way with the salt concentration. The strength of these effects depended on the nature of the anion added, increasing in the order sulfate < chloride < bromide, thus following the empirical Hofmeister series. In contrast, no significant differences were observed when changing the cation, i.e. when adding sodium or ammonium sulfate.}, language = {en} } @article{HiltlBoeker2016, author = {Hiltl, Stephanie and B{\"o}ker, Alexander}, title = {Wetting Phenomena on (Gradient) Wrinkle Substrates}, series = {Langmuir}, volume = {32}, journal = {Langmuir}, publisher = {American Chemical Society}, address = {Washington}, issn = {0743-7463}, doi = {10.1021/acs.langmuir.6b02364}, pages = {8882 -- 8888}, year = {2016}, abstract = {We characterize the wetting behavior of nano structured wrinkle and gradient wrinkle substrates. Different contact angles on both sides of a water droplet after deposition on a gradient sample induce the self-propelled motion of the liquid toward smaller wrinkle dimensions. The droplet motion is self-limited by the contact angles balancing out. Because of the correlation between droplet motion and contact angles, we investigate the wetting behavior of wrinkle substrates with constant dimensions (wavelengths of 400-1200 nm). Contact angles of water droplets on those substrates increase with increasing dimensions of the underlying substrate. The results are independent of the two measurement directions, parallel and perpendicular to the longitudinal axis of the nanostructure. The presented findings may be considered for designing microfluidic or related devices and initiate ideas for the development of further wrinkle applications.}, language = {en} } @article{HolertYuecelJagmannetal.2016, author = {Holert, Johannes and Y{\"u}cel, Onur and Jagmann, Nina and Prestel, Andreas and M{\"o}ller, Heiko Michael and Philipp, Bodo}, title = {Identification of bypass reactions leading to the formation of one central steroid degradation intermediate in metabolism of different bile salts in Pseudomonas sp strain Chol1}, series = {Environmental microbiology}, volume = {18}, journal = {Environmental microbiology}, publisher = {Wiley-Blackwell}, address = {Hoboken}, issn = {1462-2912}, doi = {10.1111/1462-2920.13192}, pages = {3373 -- 3389}, year = {2016}, language = {en} } @misc{HoogenboomSchlaad2016, author = {Hoogenboom, Richard and Schlaad, Helmut}, title = {Thermoresponsive poly(2-oxazoline)s, polypeptoids, and polypeptides}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-395022}, pages = {17}, year = {2016}, abstract = {This review covers the recent advances in the emerging field of thermoresponsive polyamides or polymeric amides, i.e., poly(2-oxazoline)s, polypeptoids, and polypeptides, with a specific focus on structure-thermoresponsive property relationships, self-assembly, and applications.}, language = {en} } @article{KathreinBaiNunnsetal.2016, author = {Kathrein, Christine C. and Bai, Wubin and Nunns, Adam and Gwyther, Jessica and Manners, Ian and B{\"o}ker, Alexander and Tsarkova, Larisa and Ross, Caroline A.}, title = {Electric field manipulated nanopatterns in thin films of metalorganic 3-miktoarm star terpolymers}, series = {Soft matter}, volume = {12}, journal = {Soft matter}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1744-683X}, doi = {10.1039/c6sm00451b}, pages = {4866 -- 4874}, year = {2016}, abstract = {We report the effect of electric field on the morphological transitions and ordering behavior of polyferrocenylethylmethylsilane block (PFEMS)-containing copolymers. By analyzing structures in solvent-annealed films of metalorganic sphere-and cylinder-forming diblock copolymers, as well as of 3-miktoarm polyisoprene-arm-polystyrene-arm-PFEMS (3 mu-ISF) terpolymers, we decouple two types of responses to the electric field: morphological transformations as a result of an increase in the volume fraction of the PFEMS block by oxidation of the ferrocenyl groups, and the orientation of the dielectric interfaces of microdomains parallel to the electric field vector. In the case of 3m-ISF, the former effect dominates at high electric field strengths which results in an unexpected cylinder-to-sphere transition, leading to a well-ordered hexagonal dot pattern. Our results demonstrate multiple tunability of ordered microdomain morphologies, suggesting future applications in nanofabrication and surface patterning.}, language = {en} } @article{KathreinPesterRuppeletal.2016, author = {Kathrein, Christine C. and Pester, Christian and Ruppel, Markus and Jung, Maike and Zimmermann, Marc and B{\"o}ker, Alexander}, title = {Reorientation mechanisms of block copolymer/CdSe quantum dot composites under application of an electric field}, series = {Soft matter}, volume = {12}, journal = {Soft matter}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1744-683X}, doi = {10.1039/c6sm01073c}, pages = {8417 -- 8424}, year = {2016}, abstract = {Time- and temperature-resolved in situ birefringence measurements were applied to analyze the effect of nanoparticles on the electric field-induced alignment of a microphase separated solution of poly(styrene)-block-poly(isoprene) in toluene. Through the incorporation of isoprene-confined CdSe quantum dots the reorientation behavior is altered. Particle loading lowers the order-disorder transition temperature, and increases the defect density, favoring nucleation and growth as an alignment mechanism over rotation of grains. The temperature dependent alteration in the reorientation mechanism is analyzed via a combination of birefringence and synchrotron SAXS. The detailed understanding of the effect of nanoparticles on the reorientation mechanism is an important prerequisite for optimization of electricfield-induced alignment of block copolymer/nanoparticle composites where the block copolymer guides the nanoparticle self-assembly into anisotropic structures.}, language = {en} } @article{KhademHilleLoehmannsroebenetal.2016, author = {Khadem, S. M. J. and Hille, Carsten and L{\"o}hmannsr{\"o}ben, Hans-Gerd and Sokolov, Igor M.}, title = {What information is contained in the fluorescence correlation spectroscopy curves, and where}, series = {Physical review : E, Statistical, nonlinear and soft matter physics}, volume = {94}, journal = {Physical review : E, Statistical, nonlinear and soft matter physics}, publisher = {American Physical Society}, address = {College Park}, issn = {2470-0045}, doi = {10.1103/PhysRevE.94.022407}, pages = {8}, year = {2016}, language = {en} } @article{KlaperWessigLinker2016, author = {Klaper, Matthias and Wessig, Pablo and Linker, Torsten}, title = {Base catalysed decomposition of anthracene endoperoxide}, series = {Chemical communications}, volume = {52}, journal = {Chemical communications}, publisher = {Royal Society of Chemistry}, address = {Cambridge}, issn = {1359-7345}, doi = {10.1039/c5cc08606j}, pages = {1210 -- 1213}, year = {2016}, abstract = {Catalytic amounts of a weak base are sufficient to induce the decomposition of anthracene endoperoxides to anthraquinone. The mechanism has been elucidated by isolation of intermediates in combination with DFT calculations. The whole process is suitable for the convenient generation of hydrogen peroxide under very mild conditions.}, language = {en} } @article{KleinpeterKoch2016, author = {Kleinpeter, Erich and Koch, Andreas}, title = {Y-aromaticity - existing: yes or no? An answer given on the magnetic criterion (TSNMRS)}, series = {Tetrahedron}, volume = {72}, journal = {Tetrahedron}, publisher = {Elsevier}, address = {Oxford}, issn = {0040-4020}, doi = {10.1016/j.tet.2016.02.020}, pages = {1675 -- 1685}, year = {2016}, abstract = {The spatial magnetic properties (Through Space NMR Shieldings - TSNMRS) of a number of Y-shaped structures possessing 4n+2 pi-electrons (i.a. the trimethylenemethane ions TMM2+, TMM2-, the guanidinium cation, substituted and hetero analogues) have been computed, visualized as Isochemical Shielding Surfaces (ICSS) of various size and direction, were examined subject to present Y-aromaticity and the results compared with energetic and geometric criteria obtained already. (C) 2016 Elsevier Ltd. All rights reserved.}, language = {en} } @phdthesis{Klier2016, author = {Klier, Dennis Tobias}, title = {Upconversion luminescence in Er-codoped NaYF4 nanoparticles}, url = {http://nbn-resolving.de/urn:nbn:de:kobv:517-opus4-98486}, school = {Universit{\"a}t Potsdam}, pages = {ix, 89}, year = {2016}, abstract = {In the context of an increasing population of aging people and a shift of medical paradigm towards an individualized medicine in health care, nanostructured lanthanides doped sodium yttrium fluoride (NaYF4) represents an exciting class of upconversion nanomaterials (UCNM) which are suitable to bring forward developments in biomedicine and -biodetection. Despite the fact that among various fluoride based upconversion (UC) phosphors lanthanide doped NaYF4 is one of the most studied upconversion nanomaterial, many open questions are still remaining concerning the interplay of the population routes of sensitizer and activator electronic states involved in different luminescence upconversion photophysics as well as the role of phonon coupling. The collective work aims to explore a detailed understanding of the upconversion mechanism in nanoscaled NaYF4 based materials co-doped with several lanthanides, e.g. Yb3+ and Er3+ as the "standard" type upconversion nanoparticles (UCNP) up to advanced UCNP with Gd3+ and Nd3+. Especially the impact of the crystal lattice structure as well as the resulting lattice phonons on the upconversion luminescence was investigated in detail based on different mixtures of cubic and hexagonal NaYF4 nanoscaled crystals. Three synthesis methods, depending on the attempt of the respective central spectroscopic questions, could be accomplished in the following work. NaYF4 based upconversion nanoparticles doped with several combination of lanthanides (Yb3+, Er3+, Gd3+ and Nd3+) were synthesized successfully using a hydrothermal synthesis method under mild conditions as well as a co-precipitation and a high temperature co-precipitation technique. Structural information were gathered by means of X-ray diffraction (XRD), electron microscopy (TEM), dynamic light scattering (DLS), Raman spectroscopy and inductively coupled plasma atomic emission spectrometry (ICP-OES). The results were discussed in detail with relation to the spectroscopic results. A variable spectroscopic setup was developed for multi parameter upconversion luminescence studies at various temperature 4 K to 328 K. Especially, the study of the thermal behavior of upconversion luminescence as well as time resolved area normalized emission spectra were a prerequisite for the detailed understanding of intramolecular deactivation processes, structural changes upon annealing or Gd3+ concentration, and the role of phonon coupling for the upconversion efficiency. Subsequently it became possible to synthesize UCNP with tailored upconversion luminescence properties. In the end, the potential of UCNP for life science application should be enunciated in context of current needs and improvements of a nanomaterial based optical sensors, whereas the "standard" UCNP design was attuned according to the special conditions in the biological matrix. In terms of a better biocompatibility due to a lower impact on biological tissue and higher penetrability for the excitation light. The first step into this direction was to use Nd3+ ions as a new sensitizer in tridoped NaYF4 based UCNP, whereas the achieved absolute and relative temperature sensitivity is comparable to other types of local temperature sensors in the literature.}, language = {en} } @article{KnightWangGallandietal.2016, author = {Knight, Joseph W. and Wang, Xiaopeng and Gallandi, Lukas and Dolgounitcheva, Olga and Ren, Xinguo and Ortiz, J. Vincent and Rinke, Patrick and K{\"o}rzd{\"o}rfer, Thomas and Marom, Noa}, title = {Accurate Ionization Potentials and Electron Affinities of Acceptor Molecules III: A Benchmark of GW Methods}, series = {Journal of chemical theory and computation}, volume = {12}, journal = {Journal of chemical theory and computation}, publisher = {American Chemical Society}, address = {Washington}, issn = {1549-9618}, doi = {10.1021/acs.jctc.5b00871}, pages = {615 -- 626}, year = {2016}, abstract = {The performance of different GW methods is assessed for a set of 24 organic acceptors. Errors are evaluated with respect to coupled cluster singles, doubles, and perturbative triples [CCSD(T)] reference data for the vertical ionization potentials (IPs) and electron affinities (EAs), extrapolated to the complete basis set limit. Additional comparisons are made to experimental data, where available. We consider fully self-consistent GW (scGW), partial self-consistency in the Green's function (scGW0), non-self-consistent G0W0 based on several mean-field starting points, and a "beyond GW" second-order screened exchange (SOSEX) correction to G0W0. We also describe the implementation of the self-consistent Coulomb hole with screened exchange method (COHSEX), which serves as one of the mean-field starting points. The best performers overall are G0W0+SOSEX and G0W0 based on an IP-tuned long-range corrected hybrid functional with the former being more accurate for EAs and the latter for IPs. Both provide a balanced treatment of localized vs delocalized states and valence spectra in good agreement with photoemission spectroscopy (PES) experiments.}, language = {en} }