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Kurtash, Vladislav; Mathew, Sobin; Thiele, Sebastian; Scheler, Theresa; Reiprich, Johannes; Hähnlein, Bernd; Stauffenberg, Jaqueline; Manske, Eberhard; Narasimha, Shilpashree; Abedin, Saadman; Jacobs, Heiko O.; Pezoldt, Jörg
Hysteresis associated with intrinsic-oxide traps in gate-tunable tetrahedral CVD-MoS2 memristor. - In: IEEE 22nd International Conference on Nanotechnology (NANO), (2022), S. 527-530

We introduce back gated memristor based on CVD-grown 30-40 nm thick MoS2 channel. The device demonstrates bipolar behaviour and the measurements are consistent with the simulations performed within the intrinsic-oxide traps model. This confirms the theory that the source of hysteresis in thin-film MoS2 memristors is charge trapping on MoS2/SiO2 interface and the grain boundaries. The impact of back gate voltage bias, voltage sweep range and channel area on memristive effect was studied and quantified using hysteresis area. Hysteresis in bipolar memristors can be tuned by back gate voltage, which makes these devices promising for neuromorphic computing.



https://doi.org/10.1109/NANO54668.2022.9928717
Zare Pour, Mohammad Amin; Romanyuk, Oleksandr; Moritz, Dominik Christian; Paszuk, Agnieszka; Maheu, Clément; Shekarabi, Sahar; Hanke, Kai Daniel; Ostheimer, David; Mayer, Thomas; Hofmann, Jan Philipp; Jaegermann, Wolfram; Hannappel, Thomas
Band energy diagrams of n-GaInP/n-AlInP(100) surfaces and heterointerfaces studied by X-ray photoelectron spectroscopy. - In: Surfaces and Interfaces, ISSN 2468-0230, Bd. 34 (2022), 102384, S. 1-7

Lattice matched n-type AlInP(100) charge selective contacts are commonly grown on n-p GaInP(100) top absorbers in high-efficiency III-V multijunction solar or photoelectrochemical cells. The cell performance can be greatly limited by the electron selectivity and valance band offset at this heterointerface. Understanding of the atomic and electronic properties of the GaInP/AlInP heterointerface is crucial for the reduction of photocurrent losses in III-V multijunction devices. In our paper, we investigated chemical composition and electronic properties of n-GaInP/n-AlInP heterostructures by X-ray photoelectron spectroscopy (XPS). To mimic an in-situ interface experiment with in-situ stepwise deposition of the contact material, 1 nm -50 nm thick n-AlInP(100) epitaxial layers were grown on n-GaInP(100) buffer layer on n-GaAs(100) substrates by metal organic vapor phase epitaxy. We observed (2 × 2)/c(4 × 2) low-energy electron diffraction patterns with characteristic diffuse streaks along the [011¯] direction due to PP dimers on both AlInP(100) and GaInP(100) as-prepared surfaces. Atomic composition analysis confirmed P-rich termination on both surfaces. Angle-resolved XPS measurements revealed a surface core level shift of 0.9 eV in P 2p peaks and the absence of interface core level shifts. We assigned the surface chemical shift in the P 2p spectrum to PP bonds on a surface. We found an upward surface band bending on the (2 × 2)/c(4 × 2) surfaces most probably caused by localized mid-gap electronic states. Pinning of the Fermi level by localized electronic states remained in n-GaInP/n-AlInP heterostructures. A valence band offset of 0.2 eV was derived by XPS and band alignment diagram models for the n-n junctions were suggested.



https://doi.org/10.1016/j.surfin.2022.102384
Koch, Juliane; Liborius, Lisa; Kleinschmidt, Peter; Weimann, Nils; Prost, Werner; Hannappel, Thomas
Electrical properties of the base-substrate junction in freestanding core-shell nanowires. - In: Advanced materials interfaces, ISSN 2196-7350, Bd. 9 (2022), 30, 2200948, S. 1-8

Well-defined hetero-interfaces with controlled properties are crucial for any high-performance, semiconductor-based, (opto-)electronic device. They are particularly important for device structures on the nanoscale with increased interfacial areas. Utilizing a ultrahigh-vacuum based multi-tip scanning tunneling microscope, this work reveals inadvertent conductivity channels between the nanowire (NW) base and the substrate, when measuring individual vertical core-shell III-V-semiconductor NWs. For that, four-terminal probing is applied on freestanding, epitaxially grown coaxial p-GaAs/i-GaInP/n-GaInP NWs without the need of nanoscale lithography or deposition of electrical contacts. This advanced analysis, carried out after composition-selective wet chemical etching, reveals a substantially degraded electrical performance of the freestanding NWs compared to detached ones. In an electron beam induced current mode of the nanosensor, charge separation at the substrate-to-NW base junction is demonstrated. An energy dispersive X-ray spectroscopic linescan shows an unintended compositional change of the epitaxially grown NW toward the planar layers caused by different incorporation mechanisms of Ga and In at the NW base. This approach provides direct insight into the NW-substrate transition area and leads to a model of the conductivity channels at the NW base, which should, in principle, be considered in the fabrication of all NW heterostructures grown bottom-up on heterogeneous substrate materials.



https://doi.org/10.1002/admi.202200948
Moritz, Dominik Christian; Ruiz Alvarado, Isaac Azahel; Zare Pour, Mohammad Amin; Paszuk, Agnieszka; Frieß, Tilo; Runge, Erich; Hofmann, Jan Philipp; Hannappel, Thomas; Schmidt, W. Gero; Jaegermann, Wolfram
P-terminated InP (001) surfaces: surface band bending and reactivity to water. - In: ACS applied materials & interfaces, ISSN 1944-8252, Bd. 14 (2022), 41, S. 47255-47261

Stable InP (001) surfaces are characterized by fully occupied and empty surface states close to the bulk valence and conduction band edges, respectively. The present photoemission data show, however, a surface Fermi level pinning only slightly below the midgap energy which gives rise to an appreciable surface band bending. By means of density functional theory calculations, it is shown that this apparent discrepancy is due to surface defects that form at finite temperature. In particular, the desorption of hydrogen from metalorganic vapor phase epitaxy grown P-rich InP (001) surfaces exposes partially filled P dangling bonds that give rise to band gap states. These defects are investigated with respect to surface reactivity in contact with molecular water by low-temperature water adsorption experiments using photoemission spectroscopy and are compared to our computational results. Interestingly, these hydrogen-related gap states are robust with respect to water adsorption, provided that water does not dissociate. Because significant water dissociation is expected to occur at steps rather than terraces, surface band bending of a flat InP (001) surface is not affected by water exposure.



https://doi.org/10.1021/acsami.2c13352
Rothe, Karl; Néel, Nicolas; Bocquet, Marie-Laure; Kröger, Jörg
Tracking the interaction between a CO-functionalized probe and two Ag-phthalocyanine conformers by local vertical force spectroscopy. - In: The journal of physical chemistry, ISSN 1520-5215, Bd. 126 (2022), 39, S. 6890-6897

Intentionally terminating scanning probes with a single atom or molecule belongs to a rapidly growing field in the quantum chemistry and physics at surfaces. However, the detailed understanding of the coupling between the probe and adsorbate is in its infancy. Here, an atomic force microscopy probe functionalized with a single CO molecule is approached with picometer control to two conformational isomers of Ag-phthalocyanine adsorbed on Ag(111). The isomer with the central Ag atom pointing to CO exhibits a complex evolution of the distance-dependent interaction, while the conformer with Ag bonded to the metal surface gives rise to a Lennard-Jones behavior. By virtue of spatially resolved force spectroscopy and the comparison with results obtained from microscope probes terminated with a single Ag atom, the mutual coupling of the protruding O atom of the tip and the Ag atom of the phthalocyanine molecule is identified as the cause for the unconventional variation of the force. Simulations of the entire junction within density functional theory unveil the presence of ample relaxations in the case of one conformer, which represents a rationale for the peculiar vertical-distance evolution of the interaction. The simulations highlight the role of physisorption, chemisorption, and unexpected junction distortions at the verge of bond formation in the interpretation of the distance-dependent force between two molecules.



https://doi.org/10.1021/acs.jpca.2c04760
Rothe, Karl; Néel, Nicolas; Bocquet, Marie-Laure; Kröger, Jörg
Extraction of chemical reactivity and structural relaxations of an organic dye from the short-range interaction with a molecular probe. - In: The journal of physical chemistry letters, ISSN 1948-7185, Bd. 13 (2022), 37, S. 8660-8665

A CO-functionalized atomic force microscope tip is used to locally probe local chemical reactivity and subtle structural relaxations of a single phthalocyanine molecule at different stages of pyrrolic-H abstraction. Spatially resolved vertical force spectroscopy unveils a variation of the maximum short-range attraction between CO and intramolecular sites, which is interpreted as a measure for the local chemical reactivity. In addition, the vertical position of the point of maximum attraction is observed to vary across the molecules. These changes follow the calculated adsorption heights of the probed molecular atoms.



https://doi.org/10.1021/acs.jpclett.2c02140
Gizatullin, Bulat; Mattea, Carlos; Shikhov, Igor; Arns, Christoph; Stapf, Siegfried
Modeling molecular interactions with wetting and non-wetting rock surfaces by combining electron paramagnetic resonance and NMR relaxometry. - In: Langmuir, ISSN 1520-5827, Bd. 38 (2022), 36, S. 11033-11053

Three types of natural rocks - Bentheimer and Berea sandstones, as well as Liège Chalk - have been aged by immersion in a bitumen solution for extended periods of time in two steps, changing the surface conditions from water-wet to oil-wet. NMR relaxation dispersion measurements were carried out on water and oil constituents, with saturated and aromatic molecules considered individually. In order to separate the different relaxation mechanisms discussed in the literature, 1H and 19F relaxation times were compared to 2H for fully deuterated liquids: while 2H relaxes predominantly by quadrupolar coupling, which is an intramolecular process, the remaining nuclei relax by dipolar coupling, which potentially consists of intra- and intermolecular contributions. The wettability change becomes evident in an increase of relaxation rates for oil and a corresponding decrease for water. However, this expected behavior dominates only for the spin-lattice relaxation rate R1 at very low field strengths and for the spin-spin relaxation rate R2, while high-field longitudinal relaxation shows a much weaker or even reverse trend. This is attributed in part to a change of radical concentration on the pore surface upon coverage of the native rock surface by bitumen as well as by the change of surface chemistry and roughness. EPR and DNP measurements quantify the change of volume vs surface radical concentration in the rocks, and an improved understanding of the role of relaxation via paramagnetic centers is obtained. By means of comparing different fluids and nuclei in combination with a defined wettability change of natural rocks, a refined model for molecular dynamics in conjunction with NMR relaxation dispersion is proposed.



https://doi.org/10.1021/acs.langmuir.2c01681
Mathew, Sobin; Narasimha, Shilpashree; Reiprich, Johannes; Scheler, Theresa; Hähnlein, Bernd; Thiele, Sebastian; Stauffenberg, Jaqueline; Kurtash, Vladislav; Abedin, Saadman; Manske, Eberhard; Jacobs, Heiko O.; Pezoldt, Jörg
Formation and characterization of three-dimensional tetrahedral MoS2 thin films by chemical vapor deposition. - In: Crystal growth & design, ISSN 1528-7505, Bd. 22 (2022), 9, S. 5229-5238

A method to synthesize the three-dimensional arrangement of bulk tetrahedral MoS2 thin films by solid source chemical vapor deposition of MoO3 and S is presented. The developed synthesizing recipe uses a temperature ramping with a constant N2 gas flow in the deposition process to grow tetrahedral MoS2 thin film layers. The study analyses the time-dependent growth morphologies, and the results are combined and presented in a growth model. A combination of optical, electron, atomic force microscopy, Raman spectroscopy, and X-ray diffraction are used to study the morphological and structural features of the tetrahedral MoS2 thin layers. The grown MoS2 is c-axis oriented 2H-MoS2. Additionally, the synthesized material is further used to fabricate back-gated field-effect transistors (FETs). The fabricated FET devices on the tetrahedral MoS2 show on/off current ratios of 10^6 and mobility up to ∼56 cm^2 V^-1 s^-1 with an estimated carrier concentration of 4 × 10^16 cm-3 for VGS = 0 V.



https://doi.org/10.1021/acs.cgd.2c00333
Calderón, Jesús A.; Tafur Sotelo, Julio C.; Barriga Gamarra, Benjamín; Alencastre, Jorge; Lozano, John; Urbizagástegui, Rodrigo; Solano, Gonzalo; Menacho, Daniel
Optimization for vibration analysis in rotating machines. - In: Renewable energy & power quality journal, ISSN 2172-038X, Bd. 20 (2022), 315, S. 369-373

A not stable mechanical movement transmission between systems produces equilibrium losses, such as a rotor of motors that are coupled in rotating machines. This can be studied as a disturbance “vibration” either as characteristic of the movement transmission due to controlled displacement over rotors, which transmits the movement. Therefore, in this research is presented an analysis for an optimal control of the rotor axis displacement that includes “vibration” as the part of the movement transmission. It implies mathematical modelling and specific sensors selections to correlate the vibration in this control task. Furthermore, in order to verify the proposed analysis, it was simulated and tested in a hybrid magnetic bearing system.



https://doi.org/10.24084/repqj20.315
Cheng, Wen-Hui; Richter, Matthias H.; Müller, Ralph; Kelzenberg, Michael; Yalamanchili, Sisir; Jahelka, Phillip R.; Perry, Andrea N.; Wu, Pin Chieh; Saive, Rebecca; Dimroth, Frank; Brunschwig, Bruce S.; Hannappel, Thomas; Atwater, Harry A.
Integrated solar-driven device with a front surface semitransparent catalysts for unassisted CO2 reduction. - In: Advanced energy materials, ISSN 1614-6840, Bd. 12 (2022), 36, 2201062, S. 1-9

Monolithic integrated photovoltaic-driven electrochemical (PV-EC) artificial photosynthesis is reported for unassisted CO2 reduction. The PV-EC structures employ triple junction photoelectrodes with a front mounted semitransparent catalyst layer as a photocathode. The catalyst layer is comprised of an array of microscale triangular metallic prisms that redirect incoming light toward open areas of the photoelectrode to reduce shadow losses. Full wave electromagnetic simulations of the prism array (PA) structure guide optimization of geometries and length scales. An integrated device is constructed with Ag catalyst prisms covering 35% of the surface area. The experimental device has close to 80% of the transmittance with a catalytic surface area equivalent 144% of the glass substrate area. Experimentally this photocathode demonstrates a direct solar-to-CO conversion efficiency of 5.9% with 50 h stability. Selective electrodeposition of Cu catalysts onto the surface of the Ag triangular prisms allows CO2 conversion to higher value products enabling demonstration of a solar-to-C2+ product efficiency of 3.1%. This design featuring structures that have a semitransparent catalyst layer on a PV-EC cell is a general solution to light loss by shadowing for front surface mounted metal catalysts, and opens a route for the development of artificial photosynthesis based on this scalable design approach.



https://doi.org/10.1002/aenm.202201062