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Upconversion NaYF4:Yb:Er nanoparticles co-doped with Gd3+ and Nd3+ for thermometry on the nanoscale
(2015)
In the present work, the upconversion luminescence properties of oleic acid capped NaYF4:Gd3+:Yb3+:Er3+ upconversion nanoparticles (UCNP) with pure β crystal phase and Nd3+ ions as an additional sensitizer were studied in the temperature range of 288 K < T < 328 K. The results of this study showed that the complex interplay of different mechanisms and effects, causing the special temperature behavior of the UCNP can be developed into thermometry on the nanoscale, e.g. to be applied in biological systems on a cellular level. The performance was improved by the use of Nd3+ as an additional dopant utilizing the cascade sensitization mechanism in tri-doped UCNP.
A multi-reference study of the byproduct formation for a ring-closed dithienylethene photoswitch
(2015)
Photodriven molecular switches are sometimes hindered in their performance by forming byproducts which act as dead ends in sequences of switching cycles, leading to rapid fatigue effects. Understanding the reaction pathways to unwanted byproducts is a prerequisite for preventing them. This article presents a study of the photochemical reaction pathways for byproduct formation in the photochromic switch 1,2-bis-(3-thienyl)-ethene. Specifically, using single- and multi-reference methods the post-deexcitation reaction towards the byproduct in the electronic ground state S0 when starting from the S1–S0 conical intersection (CoIn), is considered in detail. We find an unusual low-energy pathway, which offers the possibility for the formation of a dyotropic byproduct. Several high-energy pathways can be excluded with high probability.
What are the fundamental laws for the adsorption of charged polymers onto oppositely charged surfaces, for convex, planar, and concave geometries? This question is at the heart of surface coating applications, various complex formation phenomena, as well as in the context of cellular and viral biophysics. It has been a long-standing challenge in theoretical polymer physics; for realistic systems the quantitative understanding is however often achievable only by computer simulations. In this study, we present the findings of such extensive Monte-Carlo in silico experiments for polymer–surface adsorption in confined domains. We study the inverted critical adsorption of finite-length polyelectrolytes in three fundamental geometries: planar slit, cylindrical pore, and spherical cavity. The scaling relations extracted from simulations for the critical surface charge density sc—defining the adsorption–desorption transition—are in excellent agreement with our analytical calculations based on the ground-state analysis of the Edwards equation. In particular, we confirm the magnitude and scaling of sc for the concave interfaces versus the Debye screening length 1/k and the extent of confinement a for these three interfaces for small ka values. For large ka the critical adsorption condition approaches the known planar limit. The transition between the two regimes takes place when the radius of surface curvature or half of the slit thickness a is of the order of 1/k. We also rationalize how sc(k) dependence gets modified for semi-flexible versus flexible chains under external confinement. We examine the implications of the chain length for critical adsorption—the effect often hard to tackle theoretically—putting an emphasis on polymers inside attractive spherical cavities. The applications of our findings to some biological systems are discussed, for instance the adsorption of nucleic acids onto the inner surfaces of cylindrical and spherical viral capsids.
What are the fundamental laws for the adsorption of charged polymers onto oppositely charged surfaces, for convex, planar, and concave geometries? This question is at the heart of surface coating applications, various complex formation phenomena, as well as in the context of cellular and viral biophysics. It has been a long-standing challenge in theoretical polymer physics; for realistic systems the quantitative understanding is however often achievable only by computer simulations. In this study, we present the findings of such extensive Monte-Carlo in silico experiments for polymer–surface adsorption in confined domains. We study the inverted critical adsorption of finite-length polyelectrolytes in three fundamental geometries: planar slit, cylindrical pore, and spherical cavity. The scaling relations extracted from simulations for the critical surface charge density sc—defining the adsorption–desorption transition—are in excellent agreement with our analytical calculations based on the ground-state analysis of the Edwards equation. In particular, we confirm the magnitude and scaling of sc for the concave interfaces versus the Debye screening length 1/k and the extent of confinement a for these three interfaces for small ka values. For large ka the critical adsorption condition approaches the known planar limit. The transition between the two regimes takes place when the radius of surface curvature or half of the slit thickness a is of the order of 1/k. We also rationalize how sc(k) dependence gets modified for semi-flexible versus flexible chains under external confinement. We examine the implications of the chain length for critical adsorption—the effect often hard to tackle theoretically—putting an emphasis on polymers inside attractive spherical cavities. The applications of our findings to some biological systems are discussed, for instance the adsorption of nucleic acids onto the inner surfaces of cylindrical and spherical viral capsids.
The phase behavior of an amphiphilic block copolymer based on a poly(aspartic acid) hydrophilic block and a poly(n-butyl acrylate) hydrophobic block was investigated at the air–water and air–buffer interface. The polymer forms stable monomolecular films on both subphases. At low pH, the isotherms exhibit a plateau. Compression–expansion experiments and infrared reflection absorption spectroscopy suggest that the plateau is likely due to the formation of polymer bi- or multilayers. At high pH the films remain intact upon compression and no multilayer formation is observed. Furthermore, the mineralization of calcium phosphate beneath the monolayer was studied at different pH. The pH of the subphase and thus the polymer charge strongly affects the phase behavior of the film and the mineral formation. After 4 h of mineralization at low pH, atomic force microscopy shows smooth mineral films with a low roughness. With increasing pH the mineral films become inhomogeneous and the roughness increases. Transmission electron microscopy confirms this: at low pH a few small but uniform particles form whereas particles grown at higher pH are larger and highly agglomerated. Energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy confirm the formation of calcium phosphate. The levels of mineralization are higher in samples grown at high pH.
The phase behavior of an amphiphilic block copolymer based on a poly(aspartic acid) hydrophilic block and a poly(n-butyl acrylate) hydrophobic block was investigated at the air–water and air–buffer interface. The polymer forms stable monomolecular films on both subphases. At low pH, the isotherms exhibit a plateau. Compression–expansion experiments and infrared reflection absorption spectroscopy suggest that the plateau is likely due to the formation of polymer bi- or multilayers. At high pH the films remain intact upon compression and no multilayer formation is observed. Furthermore, the mineralization of calcium phosphate beneath the monolayer was studied at different pH. The pH of the subphase and thus the polymer charge strongly affects the phase behavior of the film and the mineral formation. After 4 h of mineralization at low pH, atomic force microscopy shows smooth mineral films with a low roughness. With increasing pH the mineral films become inhomogeneous and the roughness increases. Transmission electron microscopy confirms this: at low pH a few small but uniform particles form whereas particles grown at higher pH are larger and highly agglomerated. Energy-dispersive X-ray spectroscopy and X-ray photoelectron spectroscopy confirm the formation of calcium phosphate. The levels of mineralization are higher in samples grown at high pH.
Der Aufsatz umreißt die Wirkung von Averroes’ Bearbeitung der aristotelischen ‚Poetik‘ als argumentativer Disziplin. Beginnend mit Al-Farabi und Al-Gazali im zehnten Jahrhundert wird die ‚Poetik‘ den logischen Disziplinen des ‚Organon‘ zugerechnet. Während die Theorie eines ‚poetischen Syllogismus‘ nicht rezipiert worden ist, wurde der argumentative Status der Dichtung vom zwölften Jahrhundert an auch im lateinischen Westen bekannt. Mit unterschiedlichen Begründungen übernahmen Dominicus Gundissalinus, Vincenz von Beauvais, Albertus Magnus, Roger Bacon und Thomas von Aquin die Klassifizierung der Poetik als argumentative Disziplin. Am Ende des Aufsatzes steht ein Ausblick auf Coluccio Salutatis ‚De laboribus Herculis‘ und die humanistische Rezeption dieser Tradition.
Der Aufsatz umreißt die Wirkung von Averroes’ Bearbeitung der aristotelischen ‚Poetik‘ als argumentativer Disziplin. Beginnend mit Al-Farabi und Al-Gazali im zehnten Jahrhundert wird die ‚Poetik‘ den logischen Disziplinen des ‚Organon‘ zugerechnet. Während die Theorie eines ‚poetischen Syllogismus‘ nicht rezipiert worden ist, wurde der argumentative Status der Dichtung vom zwölften Jahrhundert an auch im lateinischen Westen bekannt. Mit unterschiedlichen Begründungen übernahmen Dominicus Gundissalinus, Vincenz von Beauvais, Albertus Magnus, Roger Bacon und Thomas von Aquin die Klassifizierung der Poetik als argumentative Disziplin. Am Ende des Aufsatzes steht ein Ausblick auf Coluccio Salutatis ‚De laboribus Herculis‘ und die humanistische Rezeption dieser Tradition.
Der Aufsatz zeigt, dass es sich bei der averroischen Bearbeitung der aristotelischen ‚Poetik‘ um eine in sich konsistente Theorie der Dichtung handelt, die allerdings mit der aristotelischen Konzeption der Dichtung nur wenig zu tun hat. Ausgehend von der Übersetzung von ‚Tragödie‘ und ‚Komödie‘ mit ‚Lob‘ und ‚Tadel‘ entwickelt Averroes einen Begriff von Dichtung als moralphilosophisches Argument zum Lob der Tugend und zum Tadel des Lasters. Im Mittelpunkt steht die Interpretation des aristotelischen Begriffs der mimesis als similitudo, das heißt als Gleichnis. Als gleichnishaftes Argument ist Dichtung nur graduell von anderen argumentativen Formen wie der demonstrativen Logik und der Rhetorik unterschieden.
Der Aufsatz zeigt, dass es sich bei der averroischen Bearbeitung der aristotelischen ‚Poetik‘ um eine in sich konsistente Theorie der Dichtung handelt, die allerdings mit der aristotelischen Konzeption der Dichtung nur wenig zu tun hat. Ausgehend von der Übersetzung von ‚Tragödie‘ und ‚Komödie‘ mit ‚Lob‘ und ‚Tadel‘ entwickelt Averroes einen Begriff von Dichtung als moralphilosophisches Argument zum Lob der Tugend und zum Tadel des Lasters. Im Mittelpunkt steht die Interpretation des aristotelischen Begriffs der mimesis als similitudo, das heißt als Gleichnis. Als gleichnishaftes Argument ist Dichtung nur graduell von anderen argumentativen Formen wie der demonstrativen Logik und der Rhetorik unterschieden.