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- ItemContributions of transported Prudhoe Bay oil field emissions to the aerosol population in Utqiaġvik, Alaska(Katlenburg-Lindau : EGU, 2017) Gunsch, Matthew J.; Kirpes, Rachel M.; Kolesar, Katheryn R.; Barrett, Tate E.; China, Swarup; Sheesley, Rebecca J.; Laskin, Alexander; Wiedensohler, Alfred; Tuch, Thomas; Pratt, Kerri A.Loss of sea ice is opening the Arctic to increasing development involving oil and gas extraction and shipping. Given the significant impacts of absorbing aerosol and secondary aerosol precursors emitted within the rapidly warming Arctic region, it is necessary to characterize local anthropogenic aerosol sources and compare to natural conditions. From August to September 2015 in Utqiaġvik (Barrow), AK, the chemical composition of individual atmospheric particles was measured by computer-controlled scanning electron microscopy with energy-dispersive X-ray spectroscopy (0.13-4 μm projected area diameter) and real-time single-particle mass spectrometry (0.2-1.5 μm vacuum aerodynamic diameter). During periods influenced by the Arctic Ocean (70 % of the study), our results show that fresh sea spray aerosol contributed ∼ 20 %, by number, of particles between 0.13 and 0.4 μm, 40-70 % between 0.4 and 1 μm, and 80-100 % between 1 and 4 μm particles. In contrast, for periods influenced by emissions from Prudhoe Bay (10 % of the study), the third largest oil field in North America, there was a strong influence from submicron (0.13-1 μm) combustion-derived particles (20-50 % organic carbon, by number; 5-10 % soot by number). While sea spray aerosol still comprised a large fraction of particles (90 % by number from 1 to 4 μm) detected under Prudhoe Bay influence, these particles were internally mixed with sulfate and nitrate indicative of aging processes during transport. In addition, the overall mode of the particle size number distribution shifted from 76 nm during Arctic Ocean influence to 27 nm during Prudhoe Bay influence, with particle concentrations increasing from 130 to 920 cm-3 due to transported particle emissions from the oil fields. The increased contributions of carbonaceous combustion products and partially aged sea spray aerosol should be considered in future Arctic atmospheric composition and climate simulations.
- ItemSingle molecule level plasmonic catalysis – a dilution study of p-nitrothiophenol on gold dimers(Cambridge : Soc., 2015) Zhang, Zhenglong; Deckert-Gaudig, Tanja; Singh, Pushkar; Deckert, VolkerSurface plasmons on isolated gold dimers can initiate intermolecular reactions of adsorbed p-nitrothiophenol. At the single molecule level when dimerization is not possible an intramolecular reaction can be observed. Experimental evidence indicates that plasmon-induced hot electrons provide the required activation energy.
- ItemA thiazolo[5,4-: D] thiazole-bridged porphyrin organic framework as a promising nonlinear optical material(London : Royal Society of Chemistry (RSC), 2019) Samal, Mahalaxmi; Valligatla, Sreeramulu; Saad, Nabil A.; Rao, M. Veeramohan; Rao, D. Narayana; Sahu, Rojalin; Biswal, Bishnu P.Porphyrin-based porous organic frameworks are an important group of materials gaining interest due to their structural diversity and distinct opto-electronic properties. However, these materials are seldom explored for nonlinear optical (NLO) applications. In this work, we investigate a thiazolo[5,4-d]thiazole-bridged porous, porphyrin framework (Por-TzTz-POF) with promising NLO properties. The planar TzTz moiety coupled with integrated porphyrin units enables efficient π-conjugation and charge distribution in the Por-TzTz-POF resulting in a high nonlinear absorption coefficient (β = 1100 cm GW-1) with figure of merit (FoM) σ1/σ0 = 5571, in contrast to analogous molecules and material counterparts e.g. metal-organic frameworks (MOFs; β = ∼0.3-0.5 cm GW-1), molecular porphyrins (β = ∼100-400 cm GW-1), graphene (β = 900 cm GW-1), and covalent organic frameworks (Por-COF-HH; β = 1040 cm GW-1 and FoM = 3534). This journal is © The Royal Society of Chemistry.
- ItemOberflächenmorphologie von Arzneistoffpartikeln - Ein optisch evaluierbares Kriterium für die Auflösungsgeschwindigkeit(München : Elsevier, Urban & Fischer , 2002) Diebold, Steffen M.Für die Auflösungsgeschwindigkeit von schwer wasserlöslichen Arzneistoffpartikeln spielt die Hydrodynamik an den Partikel-Oberflächen eine große Rolle. Diese ist ihrerseits beeinflußt von der Geometrie und der Oberflächenmorphologie der Partikel. In dieser Arbeit wurde gezeigt, dass sich zur Charakterisierung dieser Parameter die Rasterelektronenmikroskopie (SEM) auch für die Untersuchung von Arzneistoffen gut eignet. Am Beispiel von Felodipin-Kristallen wurde nachgewiesen, dass reale Arzneistoffpulver auch an scheinbar „glatten“ Oberflächen Protrusionen, Kanten und Kavitäten aufweisen. Deren Größenordnungen lassen sich mit Hilfe der Elektronenmikroskopie abschätzen. Die Oberflächenmorphologie von Arzneistoffpartikeln ist ein Kriterium für die Auflösungsgeschwindigkeit oral verabreichter Arzneistoffe. Die Rasterelektronenmikroskopie leistet dabei wertvolle Dienste zur Charakterisierung der Oberflächen von Arzneistoffpartikeln.
- ItemScanning electron microscopy preparation of the cellular actin cortex: A quantitative comparison between critical point drying and hexamethyldisilazane drying(San Francisco, California, US : PLOS, 2021) Schu, Moritz; Terriac, Emmanuel; Koch, Marcus; Paschke, Stephan; Lautenschläger, Franziska; Flormann, Daniel A.D.The cellular cortex is an approximately 200-nm-thick actin network that lies just beneath the cell membrane. It is responsible for the mechanical properties of cells, and as such, it is involved in many cellular processes, including cell migration and cellular interactions with the environment. To develop a clear view of this dense structure, high-resolution imaging is essential. As one such technique, electron microscopy, involves complex sample preparation procedures. The final drying of these samples has significant influence on potential artifacts, like cell shrinkage and the formation of artifactual holes in the actin cortex. In this study, we compared the three most used final sample drying procedures: critical-point drying (CPD), CPD with lens tissue (CPD-LT), and hexamethyldisilazane drying. We show that both hexamethyldisilazane and CPD-LT lead to fewer artifactual mesh holes within the actin cortex than CPD. Moreover, CPD-LT leads to significant reduction in cell height compared to hexamethyldisilazane and CPD. We conclude that the final drying procedure should be chosen according to the reduction in cell height, and so CPD-LT, or according to the spatial separation of the single layers of the actin cortex, and so hexamethyldisilazane.
- ItemGraphene oxide functional nanohybrids with magnetic nanoparticles for improved vectorization of doxorubicin to neuroblastoma cells(Basel : MDPI AG, 2019) Lerra, L.; Farfalla, A.; Sanz, B.; Cirillo, G.; Vittorio, O.; Voli, F.; Grand, M.L.; Curcio, M.; Nicoletta, F.P.; Dubrovska, A.; Hampel, S.; Iemma, F.; Goya, G.F.With the aim to obtain a site-specific doxorubicin (DOX) delivery in neuroblastoma SH-SY5Y cells, we designed an hybrid nanocarrier combining graphene oxide (GO) and magnetic iron oxide nanoparticles (MNPs), acting as core elements, and a curcumin–human serum albumin conjugate as functional coating. The nanohybrid, synthesized by redox reaction between the MNPs@GO system and albumin bioconjugate, consisted of MNPs@GO nanosheets homogeneously coated by the bioconjugate as verified by SEM investigations. Drug release experiments showed a pH-responsive behavior with higher release amounts in acidic (45% at pH 5.0) vs. neutral (28% at pH 7.4) environments. Cell internalization studies proved the presence of nanohybrid inside SH-SY5Y cytoplasm. The improved efficacy obtained in viability assays is given by the synergy of functional coating and MNPs constituting the nanohybrids: while curcumin moieties were able to keep low DOX cytotoxicity levels (at concentrations of 0.44–0.88 µM), the presence of MNPs allowed remote actuation on the nanohybrid by a magnetic field, increasing the dose delivered at the target site.
- ItemTailor-made nanostructures bridging chaos and order for highly efficient white organic light-emitting diodes(London : Nature Publishing Group, 2019) Li, Y.; Kovačič, M.; Westphalen, J.; Oswald, S.; Ma, Z.; Hänisch, C.; Will, P.-A.; Jiang, L.; Junghaehnel, M.; Scholz, R.; Lenk, S.; Reineke, S.Organic light-emitting diodes (OLEDs) suffer from notorious light trapping, resulting in only moderate external quantum efficiencies. Here, we report a facile, scalable, lithography-free method to generate controllable nanostructures with directional randomness and dimensional order, significantly boosting the efficiency of white OLEDs. Mechanical deformations form on the surface of poly(dimethylsiloxane) in response to compressive stress release, initialized by reactive ions etching with periodicity and depth distribution ranging from dozens of nanometers to micrometers. We demonstrate the possibility of independently tuning the average depth and the dominant periodicity. Integrating these nanostructures into a two-unit tandem white organic light-emitting diode, a maximum external quantum efficiency of 76.3% and a luminous efficacy of 95.7 lm W−1 are achieved with extracted substrate modes. The enhancement factor of 1.53 ± 0.12 at 10,000 cd m−2 is obtained. An optical model is built by considering the dipole orientation, emitting wavelength, and the dipole position on the sinusoidal nanotexture.
- ItemDeformation characteristics of solid-state benzene as a step towards understanding planetary geology([London] : Nature Publishing Group UK, 2022) Zhang, Wenxin; Zhang, Xuan; Edwards, Bryce W.; Zhong, Lei; Gao, Huajian; Malaska, Michael J.; Hodyss, Robert; Greer, Julia R.Small organic molecules, like ethane and benzene, are ubiquitous in the atmosphere and surface of Saturn’s largest moon Titan, forming plains, dunes, canyons, and other surface features. Understanding Titan’s dynamic geology and designing future landing missions requires sufficient knowledge of the mechanical characteristics of these solid-state organic minerals, which is currently lacking. To understand the deformation and mechanical properties of a representative solid organic material at space-relevant temperatures, we freeze liquid micro-droplets of benzene to form ~10 μm-tall single-crystalline pyramids and uniaxially compress them in situ. These micromechanical experiments reveal contact pressures decaying from ~2 to ~0.5 GPa after ~1 μm-reduction in pyramid height. The deformation occurs via a series of stochastic (~5-30 nm) displacement bursts, corresponding to densification and stiffening of the compressed material during cyclic loading to progressively higher loads. Molecular dynamics simulations reveal predominantly plastic deformation and densified region formation by the re-orientation and interplanar shear of benzene rings, providing a two-step stiffening mechanism. This work demonstrates the feasibility of in-situ cryogenic nanomechanical characterization of solid organics as a pathway to gain insights into the geophysics of planetary bodies.
- ItemReversibly growing crosslinked polymers with programmable sizes and properties([London] : Nature Publishing Group UK, 2023) Zhou, Xiaozhuang; Zheng, Yijun; Zhang, Haohui; Yang, Li; Cui, Yubo; Krishnan, Baiju P.; Dong, Shihua; Aizenberg, Michael; Xiong, Xinhong; Hu, Yuhang; Aizenberg, Joanna; Cui, JiaxiGrowth constitutes a powerful method to post-modulate materials’ structures and functions without compromising their mechanical performance for sustainable use, but the process is irreversible. To address this issue, we here report a growing-degrowing strategy that enables thermosetting materials to either absorb or release components for continuously changing their sizes, shapes, compositions, and a set of properties simultaneously. The strategy is based on the monomer-polymer equilibrium of networks in which supplying or removing small polymerizable components would drive the networks toward expansion or contraction. Using acid-catalyzed equilibration of siloxane as an example, we demonstrate that the size and mechanical properties of the resulting silicone materials can be significantly or finely tuned in both directions of growth and decomposition. The equilibration can be turned off to yield stable products or reactivated again. During the degrowing-growing circle, material structures are selectively varied either uniformly or heterogeneously, by the availability of fillers. Our strategy endows the materials with many appealing capabilities including environment adaptivity, self-healing, and switchability of surface morphologies, shapes, and optical properties. Since monomer-polymer equilibration exists in many polymers, we envision the expansion of the presented strategy to various systems for many applications.
- ItemUniversal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces([London] : Nature Publishing Group UK, 2017) Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, LucioSurface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.
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