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- ItemElectron Transport across Vertical Silicon/MoS2/Graphene Heterostructures: Towards Efficient Emitter Diodes for Graphene Base Hot Electron Transistors(Washington, DC : ACS Publications, 2020) Belete, Melkamu; Engström, Olof; Vaziri, Sam; Lippert, Gunther; Lukosius, Mindaugas; Kataria, Satender; Lemme, Max C.Heterostructures comprising silicon, molybdenum disulfide (MoS2), and graphene are investigated with respect to the vertical current conduction mechanism. The measured current-voltage (I-V) characteristics exhibit temperature-dependent asymmetric current, indicating thermally activated charge carrier transport. The data are compared and fitted to a current transport model that confirms thermionic emission as the responsible transport mechanism across devices. Theoretical calculations in combination with the experimental data suggest that the heterojunction barrier from Si to MoS2 is linearly temperature-dependent for T = 200-300 K with a positive temperature coefficient. The temperature dependence may be attributed to a change in band gap difference between Si and MoS2, strain at the Si/MoS2 interface, or different electron effective masses in Si and MoS2, leading to a possible entropy change stemming from variation in density of states as electrons move from Si to MoS2. The low barrier formed between Si and MoS2 and the resultant thermionic emission demonstrated here make the present devices potential candidates as the emitter diode of graphene base hot electron transistors for future high-speed electronics. Copyright © 2020 American Chemical Society.
- ItemPolymer Brush-Functionalized Chitosan Hydrogels as Antifouling Implant Coatings(Columbus, Ohio : American Chemical Society, 2017) Buzzacchera, Irene; Vorobii, Mariia; Kostina, Nina Yu; de Los Santos Pereira, Andres; Riedel, Tomáš; Bruns, Michael; Ogieglo, Wojciech; Möller, Martin; Wilson, Christopher J.; Rodriguez-Emmenegger, CesarImplantable sensor devices require coatings that efficiently interface with the tissue environment to mediate biochemical analysis. In this regard, bioinspired polymer hydrogels offer an attractive and abundant source of coating materials. However, upon implantation these materials generally elicit inflammation and the foreign body reaction as a consequence of protein fouling on their surface and concomitant poor hemocompatibility. In this report we investigate a strategy to endow chitosan hydrogel coatings with antifouling properties by the grafting of polymer brushes in a "grafting-from" approach. Chitosan coatings were functionalized with polymer brushes of oligo(ethylene glycol) methyl ether methacrylate and 2-hydroxyethyl methacrylate using photoinduced single electron transfer living radical polymerization and the surfaces were thoroughly characterized by XPS, AFM, water contact angle goniometry, and in situ ellipsometry. The antifouling properties of these new bioinspired hydrogel-brush coatings were investigated by surface plasmon resonance. The influence of the modifications to the chitosan on hemocompatibility was assessed by contacting the surfaces with platelets and leukocytes. The coatings were hydrophilic and reached a thickness of up to 180 nm within 30 min of polymerization. The functionalization of the surface with polymer brushes significantly reduced the protein fouling and eliminated platelet activation and leukocyte adhesion. This methodology offers a facile route to functionalizing implantable sensor systems with antifouling coatings that improve hemocompatibility and pave the way for enhanced device integration in tissue.
- 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.
- ItemCharge transfer to ground-state ions produces free electrons([London] : Nature Publishing Group UK, 2017) You, D.; Fukuzawa, H.; Sakakibara, Y.; Takanashi, T.; Ito, Y.; Maliyar, G G.; Motomura, K.; Nagaya, K.; Nishiyama, T.; Asa, K.; Sato, Y.; Saito, N.; Oura, M.; Schöffler, M.; Kastirke, G.; Hergenhahn, U.; Stumpf, V.; Gokhberg, K.; Kuleff, A.I.; Cederbaum, L.S.; Ueda, KInner-shell ionization of an isolated atom typically leads to Auger decay. In an environment, for example, a liquid or a van der Waals bonded system, this process will be modified, and becomes part of a complex cascade of relaxation steps. Understanding these steps is important, as they determine the production of slow electrons and singly charged radicals, the most abundant products in radiation chemistry. In this communication, we present experimental evidence for a so-far unobserved, but potentially very important step in such relaxation cascades: Multiply charged ionic states after Auger decay may partially be neutralized by electron transfer, simultaneously evoking the creation of a low-energy free electron (electron transfer-mediated decay). This process is effective even after Auger decay into the dicationic ground state. In our experiment, we observe the decay of Ne2+ produced after Ne 1s photoionization in Ne-Kr mixed clusters.