Publications at the Department of Mathematics and Natural Sciences from 2019

Results: 902
Created on: Mon, 06 May 2024 23:11:01 +0200 in 0.0928 sec


Ruiz Alvarado, Isaac Azahel; Karmo, Marsel; Runge, Erich; Schmidt, W. Gero
InP and AlInP(001)(2 × 4) surface oxidation from density functional theory. - In: ACS omega, ISSN 2470-1343, Bd. 6 (2021), 9, S. 6297-6304

The atomic structure and electronic properties of the InP and Al0.5In0.5P(001) surfaces at the initial stages of oxidation are investigated via density functional theory. Thereby, we focus on the mixed-dimer (2 × 4) surfaces stable for cation-rich preparation conditions. For InP, the top In-P dimer is the most favored adsorption site, while it is the second-layer Al-Al dimer for AlInP. The energetically favored adsorption sites yield group III-O bond-related states in the energy region of the bulk band gap, which may act as recombination centers. Consistently, the In p state density around the conduction edge is found to be reduced upon oxidation.



https://doi.org/10.1021/acsomega.0c06019
Néel, Nicolas; Kröger, Jörg
Atomic force extrema induced by the bending of a CO-functionalized probe. - In: Nano letters, ISSN 1530-6992, Bd. 21 (2021), 5, S. 2318-2323

The control and observation of reactants forming a chemical bond at the single-molecule level is a long-standing challenge in quantum physics and chemistry. Using a single CO molecule adsorbed at the apex of an atomic force microscope tip together with a Cu(111) surface, bending of the molecular probe is induced by torques due to van der Waals attraction and Pauli repulsion. As a result, the vertical force between CO and Cu(111) exhibits a characteristic dip-hump evolution with the molecule-surface separation, which depends sensitively on the initial tilt angle the CO axis encloses with the surface normal. The experimental force data are reproduced by model calculations that consider the CO deflection in a harmonic potential and the molecular orientation in the Pauli repulsion term of the Lennard-Jones potential. The presented findings shed new light on vertical-force extrema that can occur in scanning probe experiments with functionalized tips.



https://doi.org/10.1021/acs.nanolett.1c00268
Xu, C.; Zhan, Jing; Wang, Z.; Fang, X.; Chen, J.; Liang, Feng; Zhao, Huaping; Lei, Yong
Biomass-derived highly dispersed Co/Co9S8 nanoparticles encapsulated in S, N-co-doped hierarchically porous carbon as an efficient catalyst for hybrid Na-CO2 batteries. - In: Materials today, ISSN 2468-6069, Bd. 19 (2021), 100594, insges. 12 S.
Im Titel sind "9", "8" und "2" tiefgestellt

Na-CO2 batteries are prospective in energy storage and CO2 recycling applications; development of a high-efficiency, low-cost electrocatalyst to promote CO2 reduction and carbonate decomposition is extremely vital for practical Na-CO2 batteries. Herein, a highly efficient cathode catalyst for rechargeable hybrid Na-CO2 batteries is successfully synthesized by encapsulating highly dispersed Co/Co9S8 nanoparticles into carbon skeletons, consisting of biomass-derived S, N-co-doped hierarchically porous carbon (Co/Co9S8SNHC). The conductive and hierarchically porous framework structure of the Co/Co9S8@SNHC can not only accelerate electron transport, electrolyte infiltration, and CO2 diffusion but also can inhibit overgrowth and agglomeration of Co/Co9S8 nanoparticles and expose numerous high density of active sites, as well as offer sufficient space to store discharge products. Benefiting from the synergistic effect among S and N dopants, carbon defects, and Co/Co9S8 nanoparticles in robust porous carbon structure, the hybrid Na-CO2 batteries displayed a low charge overpotential (only ˜0.32 V) at 0.2 mA/cm2 and repeatedly charged and discharged over 200 cycles at 0.1 mA/cm2. Besides, an ultrahigh areal capacity of ˜18.9 mAh/cm2 was obtained at 0.5 mA/cm2, the highest value to date for Na-CO2 batteries. Meanwhile, the hybrid Na-CO2 battery charging from Na2CO3@C catalytic cathode demonstrated the high catalytic activity of biomass-derived S,N-co-doped hierarchically porous carbon (Co/Co9S8@SNHC) for CO2 reduction and carbonate decomposition. Given this finding, this work might open up a potential avenue for the reasonable design of low-cost and highly efficient catalysts for advanced metal-CO2 batteries systems.



https://doi.org/10.1016/j.mtener.2020.100594
Duan, Yu; Feng, Shuanglong; Guo, Shenghui; Gao, Jiyun; Qiu, Jiajia; Yang, Li
Efficient and inexpensive MPCVD method to synthesize Co3O4/MoS2 heterogeneous composite materials with high stability for supercapacitors. - In: Journal of materials research and technology, ISSN 2214-0697, Bd. 10 (2021), S. 953-959

Large-sized metal oxide particles have the potential to constitute cheap, high-performance, and high-stability supercapacitor electrode materials. Herein, the marketable large-sized Co3O4 particles (˜6 [my]m) as the starting raw material, inexpensive Co3O4/MoS2 core-shell heterogeneous composites have been one-step fabricated via an improvised MPCVD system modified by a domestic microwave oven. After that, the surface morphology, composition structure, and valence state of elements were analyzed to the confirmed successful synthesis of MoS2 on the surface of Co3O4. Besides, the performance was tested by cyclic voltammetry and galvanostatic charge-discharge method. The results show that the synergistic effect of Co3O4 core and MoS2 shell can effectively improve the material's electrochemical performance. The specific capacitance of Co3O4/MoS2 composite can reach 337 F g^-1 with a current density of 0.5 A g^-1, which is six times more than the raw Co3O4 powder. Furthermore, it could maintain 93.6% of the initial specific capacitance after 2000 charges and discharges. Finally, the mechanism of material performance improvement is proposed.



https://doi.org/10.1016/j.jmrt.2020.12.101
Huo, Dexian; Chen, Bin; Li, Mingtao; Meng, Guowen; Lei, Yong; Zhu, Chuhong
Template-assisted fabrication of Ag-nanoparticlesZnO-nanorods array as recyclable 3D surface enhanced Raman scattering substrate for rapid detection of trace pesticides. - In: Nanotechnology, ISSN 1361-6528, Bd. 32 (2021), 14, 145302, S. 1-9

We present a template-assisted fabrication method for a large-scale ordered arrays of ZnO nanorods (ZnO-NRs) modified with Ag nanoparticles (Ag-NPs), which possess high-density three-dimensional (3D) hot spots uniformly dispersed all over the substrate, being beneficial to ultrahigh sensitivity of surface enhanced Raman scattering (SERS) detection. These achieved Ag-NPsZnO-NRs arrays show high sensitivity, good spectral uniformity and reproducibility as substrates for SERS detection. Using the arrays, both dye molecules (rhodamine 6G, R6G) and organic pollutants like toxic pesticides (thiram and methyl parathion) are detected, with the detection limits of thiram and methyl parathion being 0.79 x 10^-9 M and 1.51 x 10^-8 M, respectively. In addition, the Ag-NPs@ZnO-NRs arrays have a self-cleaning function because the analyte molecules can be photocatalytic degraded using ultraviolet irradiation, showing that the 3D recyclable arrays have promising opportunities to be applied in rapid SERS-based detection of toxic organic pesticides.



https://doi.org/10.1088/1361-6528/abc50e
Bang-Jensen, Jørgen; Bessy, Stéphane; Huang, Jing; Kriesell, Matthias
Good orientations of unions of edge-disjoint spanning trees. - In: Journal of graph theory, ISSN 1097-0118, Bd. 96 (2021), 4, S. 594-618

In this paper, we exhibit connections between the following subjects: Tree packing in graphs and digraphs (both behave completely different), the rigidity matroid of a graph, Henneberg moves on trees, the conjectures of Thomassen and Matthews and Sumner, and (s,t)-orderings of digraphs. We do this by studying graphs which admit acyclic orientations that contain an out-branching and in-branching which are arc-disjoint (such an orientation is called good). A 2T-graph is a graph whose edge set can be decomposed into two edge-disjoint spanning trees. It is a well-known result due to Tutte and Nash-Williams, respectively, that every 4-edge-connected graph contains a spanning 2T-graph. Vertex-minimal 2T-graphs with at least two vertices which are known as generic circuits play an important role in rigidity theory for graphs. We prove that every generic circuit has a good orientation. Using this result we prove that if G is 2T-graph whose vertex set has a partition V1,V2, ,Vk so that each Vi induces a generic circuit Gi of G and the set of edges between different Gi's form a matching in G, then G has a good orientation. We also obtain a characterization for the case when the set of edges between different Gi's form a double tree, that is, if we contract each Gi to one vertex, and delete parallel edges we obtain a tree. All our proofs are constructive and imply polynomial algorithms for finding the desired good orderings and the pairs of arc-disjoint branchings which certify that the orderings are good. We identify a structure which can be used to certify that a given 2T-graph does not have a good orientation.



https://doi.org/10.1002/jgt.22633
Meier, Lukas; Braun, Christian; Hannappel, Thomas; Schmidt, W. Gero
Band alignment at GaxIn1-xP/AlyIn1-yP alloy interfaces from hybrid density functional theory calculations. - In: Physica status solidi, ISSN 1521-3951, Bd. 258 (2021), 2, 2000463, insges. 4 S.

The composition dependence of the natural band alignment at the GaxIn1-xP/AlyIn1-yP alloy interface is investigated via hybrid functional based density functional theory. The direct-indirect crossover for the GaxIn1-xP and AlyIn1-yP alloys is calculated to occur for x = 0.9 and y = 0.43. The calculated GaxIn1-xP/AlyIn1-yP interface band alignment shows a crossover from type-I to type-II with increasing Ga content x. The valence band offset is essentially positive irrespective of the alloy compositions, and amounts up to 0.56 eV. The conduction band offset varies between −0.85 and 1.16 eV.



https://doi.org/10.1002/pssb.202000463
Visaveliya, Nikunjkumar R.; Köhler, Michael
Hierarchical assemblies of polymer particles through tailored interfaces and controllable interfacial interactions. - In: Advanced functional materials, ISSN 1616-3028, Bd. 31 (2021), 9, 2007407, insges. 22 S.

Hierarchical assembly architectures of functional polymer particles are promising because of their physicochemical and surface properties for multi-labeling and sensing to catalysis and biomedical applications. While polymer nanoparticles' interior is mainly made up of the cross-linked network, their surface can be tailored with soft, flexible, and responsive molecules and macromolecules as potential support for the controlled particulate assemblies. Molecular surfactants and polyelectrolytes as interfacial agents improve the stability of the nanoparticles whereas swellable and soft shell-like cross-linked polymeric layer at the interface can significantly enhance the uptake of guest nano-constituents during assemblies. Besides, layer-by-layer surface-functionalization holds the ability to provide a high variability in assembly architectures of different interfacial properties. Considering these aspects, various assembly architectures of polymer nanoparticles of tunable size, shapes, morphology, and tailored interfaces together with controllable interfacial interactions are constructed here. The microfluidic-mediated platform has been used for the synthesis of constituents polymer nanoparticles of various structural and interfacial properties, and their assemblies are conducted in batch or flow conditions. The assemblies presented in this progress report is divided into three main categories: cross-linked polymeric network's fusion-based self-assembly, electrostatic-driven assemblies, and assembly formed by encapsulating smaller nanoparticles into larger microparticles.



https://doi.org/10.1002/adfm.202007407
Gizatullin, Bulat; Mattea, Carlos; Stapf, Siegfried
Field-cycling NMR and DNP - a friendship with benefits. - In: Journal of magnetic resonance, ISSN 1096-0856, Bd. 322 (2021), 106851, S. 1-16

Field-cycling relaxometry, or rather its electronic version with a resistive magnet which requires signal detection at a field strength of 1 Tesla or below, remains an inherently insensitive technique due to the construction compromise that goes along with the need for a fast-switching, low-inductance magnet. For the same reasons, signal lifetime is short and frequency resolution is typically not given, at least for the predominantly used hydrogen nuclei. Dynamic Nuclear Polarization (DNP) bears the potential to circumvent these disadvantages: not only has it been demonstrated to enhance magnetization by up to three orders of magnitude beyond its thermal value, but it also provides the possibility to address particular parts of a molecule, thus generating selectivity even in the absence of spectral resolution. At the same time, DNP requires the introduction of stable radicals giving rise to additional relaxation contributions. This article presents a straightforward way to recover the native relaxation rates of the undisturbed system, and shows examples in different research fields where field-cycling relaxometry is traditionally used for refining models of molecular dynamics and interactions.



https://doi.org/10.1016/j.jmr.2020.106851
Baidiuk, Dmytro; Derkach, Volodymyr; Hassi, Seppo
Unitary boundary pairs for isometric operators in Pontryagin spaces and generalized coresolvents. - In: Complex analysis and operator theory, ISSN 1661-8262, Bd. 15 (2021), 2, 32, insges. 52 S.

https://doi.org/10.1007/s11785-020-01073-4