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Saturation of the anomalous Hall effect at high magnetic fields in altermagnetic RuO2

2023, Tschirner, Teresa, Keßler, Philipp, Gonzalez Betancourt, Ruben Dario, Kotte, Tommy, Kriegner, Dominik, Büchner, Bernd, Dufouleur, Joseph, Kamp, Martin, Jovic, Vedran, Smejkal, Libor, Sinova, Jairo, Claessen, Ralph, Jungwirth, Tomas, Moser, Simon, Reichlova, Helena, Veyrat, Louis

Observations of the anomalous Hall effect in RuO2 and MnTe have demonstrated unconventional time-reversal symmetry breaking in the electronic structure of a recently identified new class of compensated collinear magnets, dubbed altermagnets. While in MnTe, the unconventional anomalous Hall signal accompanied by a vanishing magnetization is observable at remanence, the anomalous Hall effect in RuO2 is excluded by symmetry for the Néel vector pointing along the zero-field [001] easy-axis. Guided by a symmetry analysis and ab initio calculations, a field-induced reorientation of the Néel vector from the easy-axis toward the [110] hard-axis was used to demonstrate the anomalous Hall signal in this altermagnet. We confirm the existence of an anomalous Hall effect in our RuO2 thin-film samples, whose set of magnetic and magneto-transport characteristics is consistent with the earlier report. By performing our measurements at extreme magnetic fields up to 68 T, we reach saturation of the anomalous Hall signal at a field Hc ≃ 55 T that was inaccessible in earlier studies but is consistent with the expected Néel-vector reorientation field.

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Interlaboratory study assessing the analysis of supercapacitor electrochemistry data

2023, Gittins, Jamie W., Chen, Yuan, Arnold, Stefanie, Augustyn, Veronica, Balducci, Andrea, Brousse, Thierry, Frackowiak, Elzbieta, Gómez-Romero, Pedro, Kanwade, Archana, Köps, Lukas, Jha, Plawan Kumar, Lyu, Dongxun, Meo, Michele, Pandey, Deepak, Pang, Le, Presser, Volker, Rapisarda, Mario, Rueda-García, Daniel, Saeed, Saeed, Shirage, Parasharam M., Ślesiński, Adam, Soavi, Francesca, Thomas, Jayan, Titirici, Maria-Magdalena, Wang, Hongxia, Xu, Zhen, Yu, Aiping, Zhang, Maiwen, Forse, Alexander C.

Supercapacitors are fast-charging energy storage devices of great importance for developing robust and climate-friendly energy infrastructures for the future. Research in this field has seen rapid growth in recent years, therefore consistent reporting practices must be implemented to enable reliable comparison of device performance. Although several studies have highlighted the best practices for analysing and reporting data from such energy storage devices, there is yet to be an empirical study investigating whether researchers in the field are correctly implementing these recommendations, and which assesses the variation in reporting between different laboratories. Here we address this deficit by carrying out the first interlaboratory study of the analysis of supercapacitor electrochemistry data. We find that the use of incorrect formulae and researchers having different interpretations of key terminologies are major causes of variability in data reporting. Furthermore we highlight the more significant variation in reported results for electrochemical profiles showing non-ideal capacitive behaviour. From the insights gained through this study, we make additional recommendations to the community to help ensure consistent reporting of performance metrics moving forward.

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Remarkable performance recovery in highly defective perovskite solar cells by photo-oxidation

2023, Goetz, Katelyn P., Thome, Fabian T. F., An, Qingzhi, Hofstetter, Yvonne J., Schramm, Tim, Yangui, Aymen, Kiligaridis, Alexander, Loeffler, Markus, Taylor, Alexander D., Scheblykin, Ivan G., Vaynzof, Yana

Exposure to environmental factors is generally expected to cause degradation in perovskite films and solar cells. Herein, we show that films with certain defect profiles can display the opposite effect, healing upon exposure to oxygen under illumination. We tune the iodine content of methylammonium lead triiodide perovskite from understoichiometric to overstoichiometric and expose them to oxygen and light prior to the addition of the top layers of the device, thereby examining the defect dependence of their photooxidative response in the absence of storage-related chemical processes. The contrast between the photovoltaic properties of the cells with different defects is stark. Understoichiometric samples indeed degrade, demonstrating performance at 33% of their untreated counterparts, while stoichiometric samples maintain their performance levels. Surprisingly, overstoichiometric samples, which show low current density and strong reverse hysteresis when untreated, heal to maximum performance levels (the same as untreated, stoichiometric samples) upon the photooxidative treatment. A similar, albeit smaller-scale, effect is observed for triple cation and methylammonium-free compositions, demonstrating the general application of this treatment to state-of-the-art compositions. We examine the reasons behind this response by a suite of characterization techniques, finding that the performance changes coincide with microstructural decay at the crystal surface, reorientation of the bulk crystal structure for the understoichiometric cells, and a decrease in the iodine-to-lead ratio of all films. These results indicate that defect engineering is a powerful tool to manipulate the stability of perovskite solar cells.

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Degradation analysis of tribologically loaded carbon nanotubes and carbon onions

2023, MacLucas, T., Grützmacher, P., Husmann, S., Schmauch, J., Keskin, S., Suarez, S., Presser, V., Gachot, C., Mücklich, F.

Coating laser-patterned stainless-steel surfaces with carbon nanotubes (CNT) or carbon onions (CO) forms a tribological system that provides effective solid lubrication. Lubricant retention represents the fundamental mechanism of this system, as storing the particles inside the pattern prevents lubricant depletion in the contact area. In previous works, we used direct laser interference patterning to create line patterns with three different structural depths on AISI 304 stainless-steel platelets. Electrophoretic deposition subsequently coated the patterned surfaces with either CNTs or COs. Ball-on-disc friction tests were conducted to study the effect of structural depth on the solid lubricity of as-described surfaces. The results demonstrated that the shallower the textures, the lower the coefficient of friction, regardless of the applied particle type. This follow-up study examines the carbon nanoparticles’ structural degradation after friction testing on substrates patterned with different structural depths (0.24, 0.36, and 0.77 µm). Raman characterization shows severe degradation of both particle types and is used to classify their degradation state within Ferrari’s three-stage amorphization model. It was further shown that improving CNT lubricity translates into increasing particle defectivity. This is confirmed by electron microscopy, which shows decreasing crystalline domains. Compared to CNTs, CO-derived tribofilms show even more substantial structural degradation.

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Photoluminescence Mapping over Laser Pulse Fluence and Repetition Rate as a Fingerprint of Charge and Defect Dynamics in Perovskites

2023, Rao, Shraddha M., Kiligaridis, Alexander, Yangui, Aymen, An, Qingzhi, Vaynzof, Yana, Scheblykin, Ivan G.

Defects in metal halide perovskites (MHP) are photosensitive, making the observer effect unavoidable when laser spectroscopy methods are applied. Photoluminescence (PL) bleaching and enhancement under light soaking and recovery in dark are examples of the transient phenomena that are consequent to the creation and healing of defects. Depending on the initial sample composition, environment, and other factors, the defect nature and evolution can strongly vary, making spectroscopic data analysis prone to misinterpretations. Herein, the use of an automatically acquired dependence of PL quantum yield (PLQY) on the laser pulse repetition rate and pulse fluence as a unique fingerprint of both charge carrier dynamics and defect evolution is demonstrated. A simple visual comparison of such fingerprints allows for assessment of similarities and differences between MHP samples. The study illustrates this by examining methylammonium lead triiodide (MAPbI3) films with altered stoichiometry that just after preparation showed very pronounced defect dynamics at time scale from milliseconds to seconds, clearly distorting the PLQY fingerprint. Upon weeks of storage, the sample fingerprints evolve toward the standard stoichiometric MAPbI3 in terms of both charge carrier dynamics and defect stability. Automatic PLQY mapping can be used as a universal method for assessment of perovskite sample quality.

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Cracking and associated volumetric expansion of NMC811 secondary particles

2023, Shishvan, S.S., Fleck, N.A., McMeeking, R.M., Deshpande, V.S.

Secondary particles comprising a large number of nickel-rich single crystal primary particles are extensively used as storage particles in cathodes of lithium-ion batteries. It is well-established that crack formation in secondary particles is an important degradation mode that contributes to decline in battery performance. Recent X-ray tomographic observations suggest that, at very low C-rates, concentration gradients of lithium within an NMC811 secondary particle are negligible yet cracking still occurs. Additionally, during delithiation the primary particles shrink yet a volumetric expansion of the secondary particle occurs. These observations are explained by a numerical model of distributed cracking due to the extreme anisotropy of lithiation strain of primary particles. The incompatible deformation from grain to grain induces large self-stresses even in the absence of spatial gradients in the lithium concentration. The stress state is sufficient to drive a dynamic catastrophic fracture event, and the associated kinetic energy acquired by the primary particles moves them apart (akin to an explosive event) with the carbon and binder domain surrounding each secondary particle restricting the outward motion of the primary particles. It is predicted that a volume expansion of the secondary particles on the order of 20 % accompanies cracking, in agreement with recently reported observations.

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Role of topology in compensated magnetic systems

2024, Reichlova, Helena, Kriegner, Dominik, Mook, Alexander, Althammer, Matthias, Thomas, Andy

Topology plays a crucial and multifaceted role in solid state physics, leading to a remarkable array of newly investigated materials and phenomena. In this Perspective, we provide a brief summary of well-established model materials with a particular focus on compensated magnets and highlight key phenomena that emerge due to the influence of topology in these systems. The overview covers various magneto-transport phenomena, with a particular focus on the extensively investigated anomalous magneto-transport effects. Furthermore, we look into the significance of topology in understanding elementary magnetic excitations, namely magnons, where the role of topology gained considerable attention from both theoretical and experimental perspectives. Since electrons and magnons carry energy, we explore the implications of topology in combined heat and spin transport experiments in compensated magnetic systems. At the end of each section, we highlight intriguing unanswered questions in this research direction. To finally conclude, we offer our perspective on what could be the next advancements regarding the interaction between compensated magnetism and topology.

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Semitransparent Perovskite Solar Cells with an Evaporated Ultra-Thin Perovskite Absorber

2023, Zhang, Zongbao, Ji, Ran, Jia, Xiangkun, Wang, Shu‐Jen, Deconinck, Marielle, Siliavka, Elena, Vaynzof, Yana

Metal halide perovskites are of great interest for application in semitransparent solar cells due to their tunable bandgap and high performance. However, fabricating high-efficiency perovskite semitransparent devices with high average visible transmittance (AVT) is challenging because of their high absorption coefficient. Here, a co-evaporation process is adopted to fabricate ultra-thin CsPbI3 perovskite films. The smooth surface and orientated crystal growth of the evaporated perovskite films make it possible to achieve 10 nm thin films with compact and continuous morphology without pinholes. When integrated into a p-i-n device structure of glass/ITO/PTAA/perovskite/PCBM/BCP/Al/Ag with an optimized transparent electrode, these ultra-thin layers result in an impressive open-circuit voltage (VOC) of 1.08 V and a fill factor (FF) of 80%. Consequently, a power conversion efficiency (PCE) of 3.6% with an AVT above 50% is demonstrated, which is the first report for a perovskite device of a 10 nm active layer thickness with high VOC, FF and AVT. These findings demonstrate that deposition by thermal evaporation makes it possible to form compact ultra-thin perovskite films, which are of great interest for future smart windows, light-emitting diodes, and tandem device applications.

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Influence of chemical interactions on the electronic properties of BiOI/organic semiconductor heterojunctions for application in solution-processed electronics

2023, Lapalikar, Vaidehi, Dacha, Preetam, Hambsch, Mike, Hofstetter, Yvonne J., Vaynzof, Yana, Mannsfeld, Stefan C. B., Ruck, Michael

Bismuth oxide iodide (BiOI) has been viewed as a suitable environmentally-friendly alternative to lead-halide perovskites for low-cost (opto-)electronic applications such as photodetectors, phototransistors and sensors. To enable its incorporation in these devices in a convenient, scalable, and economical way, BiOI thin films were investigated as part of heterojunctions with various p-type organic semiconductors (OSCs) and tested in a field-effect transistor (FET) configuration. The hybrid heterojunctions, which combine the respective functionalities of BiOI and the OSCs were processed from solution under ambient atmosphere. The characteristics of each of these hybrid systems were correlated with the physical and chemical properties of the respective materials using a concept based on heteropolar chemical interactions at the interface. Systems suitable for application in lateral transport devices were identified and it was demonstrated how materials in the hybrids interact to provide improved and synergistic properties. These indentified heterojunction FETs are a first instance of successful incorporation of solution-processed BiOI thin films in a three-terminal device. They show a significant threshold voltage shift and retained carrier mobility compared to pristine OSC devices and open up possibilities for future optoelectronic applications.

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Analysis of the Annealing Budget of Metal Oxide Thin-Film Transistors Prepared by an Aqueous Blade-Coating Process

2022, Tang, Tianyu, Dacha, Preetam, Haase, Katherina, Kreß, Joshua, Hänisch, Christian, Perez, Jonathan, Krupskaya, Yulia, Tahn, Alexander, Pohl, Darius, Schneider, Sebastian, Talnack, Felix, Hambsch, Mike, Reineke, Sebastian, Vaynzof, Yana, Mannsfeld, Stefan C. B.

Metal oxide (MO) semiconductors are widely used in electronic devices due to their high optical transmittance and promising electrical performance. This work describes the advancement toward an eco-friendly, streamlined method for preparing thin-film transistors (TFTs) via a pure water-solution blade-coating process with focus on a low thermal budget. Low temperature and rapid annealing of triple-coated indium oxide thin-film transistors (3C-TFTs) and indium oxide/zinc oxide/indium oxide thin-film transistors (IZI-TFTs) on a 300 nm SiO2 gate dielectric at 300 °C for only 60 s yields devices with an average field effect mobility of 10.7 and 13.8 cm2 V−1 s−1, respectively. The devices show an excellent on/off ratio (>106), and a threshold voltage close to 0 V when measured in air. Flexible MO-TFTs on polyimide substrates with AlOx dielectrics fabricated by rapid annealing treatment can achieve a remarkable mobility of over 10 cm2 V−1 s−1 at low operating voltage. When using a longer post-coating annealing period of 20 min, high-performance 3C-TFTs (over 18 cm2 V−1 s−1) and IZI-TFTs (over 38 cm2 V−1 s−1) using MO semiconductor layers annealed at 300 °C are achieved.