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- ItemBuilding Hierarchical Martensite(Weinheim : Wiley-VCH, 2020) Schwabe, Stefan; Niemann, Robert; Backen, Anja; Wolf, Daniel; Damm, Christine; Walter, Tina; Seiner, Hanuš; Heczko, Oleg; Nielsch, Kornelius; Fähler, SebastianMartensitic materials show a complex, hierarchical microstructure containing structural domains separated by various types of twin boundaries. Several concepts exist to describe this microstructure on each length scale, however, there is no comprehensive approach bridging the whole range from the nano- up to the macroscopic scale. Here, it is described for a Ni-Mn-based Heusler alloy how this hierarchical microstructure is built from scratch with just one key parameter: the tetragonal distortion of the basic building block at the atomic level. Based on this initial block, five successive levels of nested building blocks are introduced. At each level, a larger building block is formed by twinning the preceding one to minimize the relevant energy contributions locally. This naturally explains the coexistence of different types of twin boundaries. The scale-bridging approach of nested building blocks is compared with experiments in real and reciprocal space. The approach of nested building blocks is versatile as it can be applied to the broad class of functional materials exhibiting diffusionless transformations. © 2020 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemRobust Single Molecule Magnet Monolayers on Graphene and Graphite with Magnetic Hysteresis up to 28 K(Weinheim : Wiley-VCH, 2021) Spree, Lukas; Liu, Fupin; Neu, Volker; Rosenkranz, Marco; Velkos, Georgios; Wang, Yaofeng; Schiemenz, Sandra; Dreiser, Jan; Gargiani, Pierluigi; Valvidares, Manuel; Chen, Chia-Hsiang; Büchner, Bernd; Avdoshenko, Stanislav M.; Popov, Alexey A.The chemical functionalization of fullerene single molecule magnet Tb2@C80(CH2Ph) enables the facile preparation of robust monolayers on graphene and highly oriented pyrolytic graphite from solution without impairing their magnetic properties. Monolayers of endohedral fullerene functionalized with pyrene exhibit magnetic bistability up to a temperature of 28 K. The use of pyrene terminated linker molecules opens the way to devise integration of spin carrying units encapsulated by fullerene cages on graphitic substrates, be it single-molecule magnets or qubit candidates. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemPerovskite Origami for Programmable Microtube Lasing(Weinheim : Wiley-VCH, 2021) Dong, Haiyun; Saggau, Christian Niclaas; Zhu, Minshen; Liang, Jie; Duan, Shengkai; Wang, Xiaoyu; Tang, Hongmei; Yin, Yin; Wang, Xiaoxia; Wang, Jiawei; Zhang, Chunhuan; Zhao, Yong Sheng; Ma, Libo; Schmidt, Oliver G.Metal halide perovskites are promising materials for optoelectronic and photonic applications ranging from photovoltaics to laser devices. However, current perovskite devices are constrained to simple low-dimensional structures suffering from limited design freedom and holding up performance improvement and functionality upgrades. Here, a micro-origami technique is developed to program 3D perovskite microarchitectures toward a new type of microcavity laser. The design flexibility in 3D supports not only outstanding laser performance such as low threshold, tunable output, and high stability but also yields new functionalities like 3D confined mode lasing and directional emission in, for example, laser “array-in-array” systems. The results represent a significant step forward toward programmable microarchitectures that take perovskite optoelectronics and photonics into the 3D era. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH.
- ItemSemitransparent Perovskite Solar Cells with an Evaporated Ultra-Thin Perovskite Absorber(Weinheim : Wiley-VCH, 2023) Zhang, Zongbao; Ji, Ran; Jia, Xiangkun; Wang, Shu‐Jen; Deconinck, Marielle; Siliavka, Elena; Vaynzof, YanaMetal 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.
- ItemStructural Aspects of P2-Type Na0.67Mn0.6Ni0.2Li0.2O2 (MNL) Stabilization by Lithium Defects as a Cathode Material for Sodium-Ion Batteries(Weinheim : Wiley-VCH, 2021) Yang, Liangtao; Kuo, Liang-Yin; López del Amo, Juan Miguel; Nayak, Prasant Kumar; Mazzio, Katherine A.; Maletti, Sebastian; Mikhailova, Daria; Giebeler, Lars; Kaghazchi, Payam; Rojo, Teófilo; Adelhelm, PhilippA known strategy for improving the properties of layered oxide electrodes in sodium-ion batteries is the partial substitution of transition metals by Li. Herein, the role of Li as a defect and its impact on sodium storage in P2-Na0.67Mn0.6Ni0.2Li0.2O2 is discussed. In tandem with electrochemical studies, the electronic and atomic structure are studied using solid-state NMR, operando XRD, and density functional theory (DFT). For the as-synthesized material, Li is located in comparable amounts within the sodium and the transition metal oxide (TMO) layers. Desodiation leads to a redistribution of Li ions within the crystal lattice. During charging, Li ions from the Na layer first migrate to the TMO layer before reversing their course at low Na contents. There is little change in the lattice parameters during charging/discharging, indicating stabilization of the P2 structure. This leads to a solid-solution type storage mechanism (sloping voltage profile) and hence excellent cycle life with a capacity of 110 mAh g-1 after 100 cycles. In contrast, the Li-free compositions Na0.67Mn0.6Ni0.4O2 and Na0.67Mn0.8Ni0.2O2 show phase transitions and a stair-case voltage profile. The capacity is found to originate from mainly Ni3+/Ni4+ and O2-/O2-δ redox processes by DFT, although a small contribution from Mn4+/Mn5+ to the capacity cannot be excluded. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemRevealing the Various Electrochemical Behaviors of Sn4P3 Binary Alloy Anodes in Alkali Metal Ion Batteries(Weinheim : Wiley-VCH, 2021) Zhou, Junhua; Lian, Xueyu; You, Yizhou; Shi, Qitao; Liu, Yu; Yang, Xiaoqin; Liu, Lijun; Wang, Dan; Choi, Jin-Ho; Sun, Jingyu; Yang, Ruizhi; Rummeli, Mark H.Sn4P3 binary alloy anode has attracted much attention, not only because of the synergistic effect of P and Sn, but also its universal popularity in alkali metal ion batteries (AIBs), including lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), and potassium-ion batteries (PIBs). However, the alkali metal ion (A+) storage and capacity attenuation mechanism of Sn4P3 anodes in AIBs are not well understood. Herein, a combination of ex situ X-ray diffraction, transmission electron microscopy, and density functional theory calculations reveals that the Sn4P3 anode undergoes segregation of Sn and P, followed by the intercalation of A+ in P and then in Sn. In addition, differential electrochemical curves and ex situ XPS results demonstrate that the deep insertion of A+ in P and Sn, especially in P, contributes to the reduction in capacity of AIBs. Serious sodium metal dendrite growth causes further reduction in the capacity of SIBs, while in PIBs it is the unstable solid electrolyte interphase and sluggish dynamics that lead to capacity decay. Not only the failure mechanism, including structural deterioration, unstable SEI, dendrite growth, and sluggish kinetics, but also the modification strategy and systematic analysis method provide theoretical guidance for the development of other alloy-based anode materials. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemAntifreezing Hydrogel with High Zinc Reversibility for Flexible and Durable Aqueous Batteries by Cooperative Hydrated Cations(Weinheim : Wiley-VCH, 2020) Zhu, Minshen; Wang, Xiaojie; Tang, Hongmei; Wang, Jiawei; Hao, Qi; Liu, Lixiang; Li, Yang; Zhang, Kai; Schmidt, Oliver G.Hydrogels are widely used in flexible aqueous batteries due to their liquid-like ion transportation abilities and solid-like mechanical properties. Their potential applications in flexible and wearable electronics introduce a fundamental challenge: how to lower the freezing point of hydrogels to preserve these merits without sacrificing hydrogels' basic advantages in low cost and high safety. Moreover, zinc as an ideal anode in aqueous batteries suffers from low reversibility because of the formation of insulative byproducts, which is mainly caused by hydrogen evolution via extensive hydration of zinc ions. This, in principle, requires the suppression of hydration, which induces an undesirable increase in the freezing point of hydrogels. Here, it is demonstrated that cooperatively hydrated cations, zinc and lithium ions in hydrogels, are very effective in addressing the above challenges. This simple but unique hydrogel not only enables a 98% capacity retention upon cooling down to −20 °C from room temperature but also allows a near 100% capacity retention with >99.5% Coulombic efficiency over 500 cycles at −20 °C. In addition, the strengthened mechanical properties of the hydrogel under subzero temperatures result in excellent durability under various harsh deformations after the freezing process. © 2019 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemOn the Catalytic Activity of Sn Monomers and Dimers at Graphene Edges and the Synchronized Edge Dependence of Diffusing Atoms in Sn Dimers(Weinheim : Wiley-VCH, 2021) Yang, Xiaoqin; Ta, Huy Q.; Hu, Huimin; Liu, Shuyuan; Liu, Yu; Bachmatiuk, Alicja; Luo, Jinping; Liu, Lijun; Choi, Jin-Ho; Rummeli, Mark H.In this study, in situ transmission electron microscopy is performed to study the interaction between single (monomer) and paired (dimer) Sn atoms at graphene edges. The results reveal that a single Sn atom can catalyze both the growth and etching of graphene by the addition and removal of C atoms respectively. Additionally, the frequencies of the energetically favorable configurations of an Sn atom at a graphene edge, calculated using density functional theory calculations, are compared with experimental observations and are found to be in good agreement. The remarkable dynamic processes of binary atoms (dimers) are also investigated and is the first such study to the best of the knowledge. Dimer diffusion along the graphene edges depends on the graphene edge termination. Atom pairs (dimers) involving an armchair configuration tend to diffuse with a synchronized shuffling (step-wise shift) action, while dimer diffusion at zigzag edge terminations show a strong propensity to collapse the dimer with each atom diffusing in opposite directions (monomer formation). Moreover, the data reveals the role of C feedstock availability on the choice a single Sn atom makes in terms of graphene growth or etching. This study advances the understanding single atom catalytic activity at graphene edges. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemPhase Selection in Mn–Si Alloys by Fast Solid-State Reaction with Enhanced Skyrmion Stability(Weinheim : Wiley-VCH, 2021) Li, Zichao; Xie, Yufang; Yuan, Ye; Ji, Yanda; Begeza, Viktor; Cao, Lei; Hübner, René; Rebohle, Lars; Helm, Manfred; Nielsch, Kornelius; Prucnal, Slawomir; Zhou, ShengqiangB20-type transition-metal silicides or germanides are noncentrosymmetric materials hosting magnetic skyrmions, which are promising information carriers in spintronic devices. The prerequisite is to prepare thin films on technology-relevant substrates with magnetic skyrmions stabilized at a broad temperature and magnetic-field working window. A canonical example is the B20-MnSi film grown on Si substrates. However, the as-yet unavoidable contamination with MnSi1.7 occurs due to the lower nucleation temperature of this phase. In this work, a simple and efficient method to overcome this problem and prepare single-phase MnSi films on Si substrates is reported. It is based on the millisecond reaction between metallic Mn and Si using flash-lamp annealing (FLA). By controlling the FLA energy density, single-phase MnSi or MnSi1.7 or their mixture can be grown at will. Compared with bulk MnSi, the prepared MnSi films show an increased Curie temperature of up to 41 K. In particular, the magnetic skyrmions are stable over a much wider temperature and magnetic-field range than reported previously. The results constitute a novel phase selection approach for alloys and can help to enhance specific functional properties, such as the stability of magnetic skyrmions. © 2021 The Authors. Advanced Functional Materials published by Wiley-VCH GmbH
- ItemA Holistic Solution to Icing by Acoustic Waves: De-Icing, Active Anti-Icing, Sensing with Piezoelectric Crystals, and Synergy with Thin Film Passive Anti-Icing Solutions(Weinheim : Wiley-VCH, 2023) del Moral, Jaime; Montes, Laura; Rico‐Gavira, Victor Joaquin; López‐Santos, Carmen; Jacob, Stefan; Oliva‐Ramirez, Manuel; Gil‐Rostra, Jorge; Fakhfouri, Armaghan; Pandey, Shilpi; Gonzalez del Val, Miguel; Mora, Julio; García‐Gallego, Paloma; Ibáñez‐Ibáñez, Pablo Francisco; Rodríguez‐Valverde, Miguel Angel; Winkler, Andreas; Borrás, Ana; González‐Elipe, Agustin RodriguezIcing has become a hot topic both in academia and in the industry given its implications in transport, wind turbines, photovoltaics, and telecommunications. Recently proposed de-icing solutions involving the propagation of acoustic waves (AWs) at suitable substrates may open the path for a sustainable alternative to standard de-icing or anti-icing procedures. Herein, the fundamental interactions are unraveled that contribute to the de-icing and/or hinder the icing on AW-activated substrates. The response toward icing of a reliable model system consisting of a piezoelectric plate activated by extended electrodes is characterized at a laboratory scale and in an icing wind tunnel under realistic conditions. Experiments show that surface modification with anti-icing functionalities provides a synergistic response when activated with AWs. A thoughtful analysis of the resonance frequency dependence on experimental variables such as temperature, ice formation, or wind velocity demonstrates the application of AW devices for real-time monitoring of icing processes.