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- ItemAmorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu7PS6(Weinheim : Wiley-VCH, 2024) Shen, Xingchen; Ouyang, Niuchang; Huang, Yuling; Tung, Yung‐Hsiang; Yang, Chun‐Chuen; Faizan, Muhammad; Perez, Nicolas; He, Ran; Sotnikov, Andrei; Willa, Kristin; Wang, Chen; Chen, Yue; Guilmeau, EmmanuelDue to their amorphous-like ultralow lattice thermal conductivity both below and above the superionic phase transition, crystalline Cu- and Ag-based superionic argyrodites have garnered widespread attention as promising thermoelectric materials. However, despite their intriguing properties, quantifying their lattice thermal conductivities and a comprehensive understanding of the microscopic dynamics that drive these extraordinary properties are still lacking. Here, an integrated experimental and theoretical approach is adopted to reveal the presence of Cu-dominated low-energy optical phonons in the Cu-based argyrodite Cu7PS6. These phonons yield strong acoustic-optical phonon scattering through avoided crossing, enabling ultralow lattice thermal conductivity. The Unified Theory of thermal transport is employed to analyze heat conduction and successfully reproduce the experimental amorphous-like ultralow lattice thermal conductivities, ranging from 0.43 to 0.58 W m−1 K−1, in the temperature range of 100–400 K. The study reveals that the amorphous-like ultralow thermal conductivity of Cu7PS6 stems from a significantly dominant wave-like conduction mechanism. Moreover, the simulations elucidate the wave-like thermal transport mainly results from the contribution of Cu-associated low-energy overlapping optical phonons. This study highlights the crucial role of low-energy and overlapping optical modes in facilitating amorphous-like ultralow thermal transport, providing a thorough understanding of the underlying complex dynamics of argyrodites.
- ItemNd─Nd Bond in Ih and D5h Cage Isomers of Nd2@C80 Stabilized by Electrophilic CF3 Addition(Weinheim : Wiley-VCH, 2023) Yang, Wei; Velkos, Georgios; Rosenkranz, Marco; Schiemenz, Sandra; Liu, Fupin; Popov, Alexey A.Synthesis of molecular compounds with metal–metal bonds between 4f elements is recognized as one of the fascinating milestones in lanthanide metallochemistry. The main focus of such studies is on heavy lanthanides due to the interest in their magnetism, while bonding between light lanthanides remains unexplored. In this work, the Nd─Nd bonding in Nd-dimetallofullerenes as a case study of metal–metal bonding between early lanthanides is demonstrated. Combined experimental and computational study proves that pristine Nd2@C80 has an open shell structure with a single electron occupying the Nd─Nd bonding orbital. Nd2@C80 is stabilized by a one-electron reduction and further by the electrophilic CF3 addition to [Nd2@C80]−. Single-crystal X-ray diffraction reveals the formation of two Nd2@C80(CF3) isomers with D5h-C80 and Ih-C80 carbon cages, both featuring a single-electron Nd─Nd bond with the length of 3.78–3.79 Å. The mutual influence of the exohedral CF3 group and endohedral metal dimer in determining the molecular structure of the adducts is analyzed. Unlike Tb or Dy analogs, which are strong single-molecule magnets with high blocking temperature of magnetization, the slow relaxation of magnetization in Nd2@Ih-C80(CF3) is detectable via out-of-phase magnetic susceptibility only below 3 K and in the presence of magnetic field.
- ItemIn Situ Fabrication of Freestanding Single-Atom-Thick 2D Metal/Metallene and 2D Metal/ Metallene Oxide Membranes: Recent Developments(Weinheim : Wiley-VCH, 2021) Ta, Huy Q.; Mendes, Rafael G.; Liu, Yu; Yang, Xiaoqin; Luo, Jingping; Bachmatiuk, Alicja; Gemming, Thomas; Zeng, Mengqi; Fu, Lei; Liu, Lijun; Rümmeli, Mark H.In recent years, two-dimensional (2D) materials have attracted a lot of research interest as they exhibit several fascinating properties. However, outside of 2D materials derived from van der Waals layered bulk materials only a few other such materials are realized, and it remains difficult to confirm their 2D freestanding structure. Despite that, many metals are predicted to exist as 2D systems. In this review, the authors summarize the recent progress made in the synthesis and characterization of these 2D metals, so called metallenes, and their oxide forms, metallene oxides as free standing 2D structures formed in situ through the use of transmission electron microscopy (TEM) and scanning TEM (STEM) to synthesize these materials. Two primary approaches for forming freestanding monoatomic metallic membranes are identified. In the first, graphene pores as a means to suspend the metallene or metallene oxide and in the second, electron-beam sputtering for the selective etching of metal alloys or thick complex initial materials is employed to obtain freestanding single-atom-thick 2D metal. The data show a growing number of 2D metals/metallenes and 2D metal/ metallene oxides having been confirmed and point to a bright future for further discoveries of these 2D materials.
- ItemHigh-Quality Graphene Using Boudouard Reaction(Weinheim : Wiley-VCH, 2022) Grebenko, Artem K.; Krasnikov, Dmitry V.; Bubis, Anton V.; Stolyarov, Vasily S.; Vyalikh, Denis V.; Makarova, Anna A.; Fedorov, Alexander; Aitkulova, Aisuluu; Alekseeva, Alena A.; Gilshtein, Evgeniia; Bedran, Zakhar; Shmakov, Alexander N.; Alyabyeva, Liudmila; Mozhchil, Rais N.; Ionov, Andrey M.; Gorshunov, Boris P.; Laasonen, Kari; Podzorov, Vitaly; Nasibulin, Albert G.Following the game-changing high-pressure CO (HiPco) process that established the first facile route toward large-scale production of single-walled carbon nanotubes, CO synthesis of cm-sized graphene crystals of ultra-high purity grown during tens of minutes is proposed. The Boudouard reaction serves for the first time to produce individual monolayer structures on the surface of a metal catalyst, thereby providing a chemical vapor deposition technique free from molecular and atomic hydrogen as well as vacuum conditions. This approach facilitates inhibition of the graphene nucleation from the CO/CO2 mixture and maintains a high growth rate of graphene seeds reaching large-scale monocrystals. Unique features of the Boudouard reaction coupled with CO-driven catalyst engineering ensure not only suppression of the second layer growth but also provide a simple and reliable technique for surface cleaning. Aside from being a novel carbon source, carbon monoxide ensures peculiar modification of catalyst and in general opens avenues for breakthrough graphene-catalyst composite production.
- ItemCharge‐Compensated N‐Doped π ‐Conjugated Polymers: Toward both Thermodynamic Stability of N‐Doped States in Water and High Electron Conductivity(Weinheim : Wiley-VCH, 2022) Borrmann, Fabian; Tsuda, Takuya; Guskova, Olga; Kiriy, Nataliya; Hoffmann, Cedric; Neusser, David; Ludwigs, Sabine; Lappan, Uwe; Simon, Frank; Geisler, Martin; Debnath, Bipasha; Krupskaya, Yulia; Al‐Hussein, Mahmoud; Kiriy, AntonThe understanding and applications of electron-conducting π-conjugated polymers with naphtalene diimide (NDI) blocks show remarkable progress in recent years. Such polymers demonstrate a facilitated n-doping due to the strong electron deficiency of the main polymer chain and the presence of the positively charged side groups stabilizing a negative charge of the n-doped backbone. Here, the n-type conducting NDI polymer with enhanced stability of its n-doped states for prospective “in-water” applications is developed. A combined experimental–theoretical approach is used to identify critical features and parameters that control the doping and electron transport process. The facilitated polymer reduction ability and the thermodynamic stability in water are confirmed by electrochemical measurements and doping studies. This material also demonstrates a high conductivity of 10−2 S cm−1 under ambient conditions and 10−1 S cm−1 in vacuum. The modeling explains the stabilizing effects for various dopants. The simulations show a significant doping-induced “collapse” of the positively charged side chains on the core bearing a partial negative charge. This explains a decrease in the lamellar spacing observed in experiments. This study fundamentally enables a novel pathway for achieving both thermodynamic stability of the n-doped states in water and the high electron conductivity of polymers.
- ItemElucidating Structure Formation in Highly Oriented Triple Cation Perovskite Films(Weinheim : Wiley-VCH, 2023) Telschow, Oscar; Scheffczyk, Niels; Hinderhofer, Alexander; Merten, Lena; Kneschaurek, Ekaterina; Bertram, Florian; Zhou, Qi; Löffler, Markus; Schreiber, Frank; Paulus, Fabian; Vaynzof, YanaMetal halide perovskites are an emerging class of crystalline semiconductors of great interest for application in optoelectronics. Their properties are dictated not only by their composition, but also by their crystalline structure and microstructure. While significant efforts are dedicated to the development of strategies for microstructural control, significantly less is known about the processes that govern the formation of their crystalline structure in thin films, in particular in the context of crystalline orientation. This work investigates the formation of highly oriented triple cation perovskite films fabricated by utilizing a range of alcohols as an antisolvent. Examining the film formation by in situ grazing-incidence wide-angle X-ray scattering reveals the presence of a short-lived highly oriented crystalline intermediate, which is identified as FAI-PbI2-xDMSO. The intermediate phase templates the crystallization of the perovskite layer, resulting in highly oriented perovskite layers. The formation of this dimethylsulfoxide (DMSO) containing intermediate is triggered by the selective removal of N,N-dimethylformamide (DMF) when alcohols are used as an antisolvent, consequently leading to differing degrees of orientation depending on the antisolvent properties. Finally, this work demonstrates that photovoltaic devices fabricated from the highly oriented films, are superior to those with a random polycrystalline structure in terms of both performance and stability.
- ItemIntermixing-Driven Surface and Bulk Ferromagnetism in the Quantum Anomalous Hall Candidate MnBi6Te10(Weinheim : Wiley-VCH, 2023) Tcakaev, Abdul‐Vakhab; Rubrecht, Bastian; Facio, Jorge I.; Zabolotnyy, Volodymyr B.; Corredor, Laura T.; Folkers, Laura C.; Kochetkova, Ekaterina; Peixoto, Thiago R. F.; Kagerer, Philipp; Heinze, Simon; Bentmann, Hendrik; Green, Robert J.; Gargiani, Pierluigi; Valvidares, Manuel; Weschke, Eugen; Haverkort, Maurits W.; Reinert, Friedrich; van den Brink, Jeroen; Büchner, Bernd; Wolter, Anja U. B.; Isaeva, Anna; Hinkov, VladimirThe recent realizations of the quantum anomalous Hall effect (QAHE) in MnBi2Te4 and MnBi4Te7 benchmark the (MnBi2Te4)(Bi2Te3)n family as a promising hotbed for further QAHE improvements. The family owes its potential to its ferromagnetically (FM) ordered MnBi2Te4 septuple layers (SLs). However, the QAHE realization is complicated in MnBi2Te4 and MnBi4Te7 due to the substantial antiferromagnetic (AFM) coupling between the SLs. An FM state, advantageous for the QAHE, can be stabilized by interlacing the SLs with an increasing number n of Bi2Te3 quintuple layers (QLs). However, the mechanisms driving the FM state and the number of necessary QLs are not understood, and the surface magnetism remains obscure. Here, robust FM properties in MnBi6Te10 (n = 2) with Tc ≈ 12 K are demonstrated and their origin is established in the Mn/Bi intermixing phenomenon by a combined experimental and theoretical study. The measurements reveal a magnetically intact surface with a large magnetic moment, and with FM properties similar to the bulk. This investigation thus consolidates the MnBi6Te10 system as perspective for the QAHE at elevated temperatures.
- ItemTailoring Intermolecular Interactions Towards High‐Performance Thermoelectric Ionogels at Low Humidity(Weinheim : Wiley-VCH, 2022) Zhao, Wei; Sun, Tingting; Zheng, Yiwei; Zhang, Qihao; Huang, Aibin; Wang, Lianjun; Jiang, WanDevelopment of ionic thermoelectric (iTE) materials is of immense interest for efficient heat-to-electricity conversion due to their giant ionic Seebeck coefficient (Si), but challenges remain in terms of relatively small Si at low humidity, poor stretchability, and ambiguous interaction mechanism in ionogels. Herein, a novel ionogel is reported consisting of polyethylene oxide (PEO), polyethylene oxide-polypropylene oxide-polyethylene oxide (P123), and 1-ethyl-3-methylimidazolium acetate (Emim:OAC). By delicately designing the interactions between ions and polymers, the migration of anions is restricted due to their strong binding with the hydroxyl groups of polymers, while the transport of cations is facilitated through segmental motions due to the increased amorphous regions, thereby leading to enlarged diffusion difference between the cations and anions. Moreover, the plasticizing effect of P123 and Emim:OAC can increase the elongation at break. As a consequence, the ionogel exhibits excellent properties including high Si (18 mV K−1 at relative humidity of 60%), good ionic conductivity (1.1 mS cm−1), superior stretchability (787%), and high stability (over 80% retention after 600 h). These findings show a promising strategy to obtain multifunctional iTE materials by engineering the intermolecular interactions and demonstrate the great potential of ionogels for harvesting low-grade heat in human-comfortable humidity environments.
- ItemHighly Symmetric and Extremely Compact Multiple Winding Microtubes by a Dry Rolling Mechanism(Weinheim : Wiley-VCH, 2020) Moradi, Somayeh; Naz, Ehsan Saei Ghareh; Li, Guodong; Bandari, Nooshin; Bandari, Vineeth Kumar; Zhu, Feng; Wendrock, Horst; Schmidt, Oliver G.Rolled-up nanotechnology has received significant attention to self-assemble planar nanomembranes into 3D micro and nanotubular architectures. These tubular structures have been well recognized as novel building blocks in a variety of applications ranging from microelectronics and nanophotonics to microbatteries and microrobotics. However, fabrication of multiwinding microtubes with precise control over the winding interfaces, which is crucial for many complex applications, is not easy to achieve by existing materials and technologies. Here, a dry rolling approach is introduced to tackle this challenge and create tight windings in compact and highly symmetric cylindrical microstructures. This technique exploits hydrophobicity of fluorocarbon polymers and the thermal expansion mismatch of polymers and inorganic films upon thermal treatment. Quality parameters for rolled-up microtubes, against which different fabrication technologies can be benchmarked are defined. The technique offers to fabricate long freestanding multiwinding microtubes as well as hierarchical architectures incorporating rolled-up wrinkled nanomembranes. This work presents an important step forward toward the fabrication of more complex but well-controlled microtubes for advanced high-quality device architectures. © 2020 The Authors. Published by WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
- ItemElectronic Doping and Enhancement of n‐Channel Polycrystalline OFET Performance through Gate Oxide Modifications with Aminosilanes(Weinheim : Wiley-VCH, 2021) Shin, Nara; Schellhammer, Karl Sebastian; Lee, Min Ho; Zessin, Jakob; Hambsch, Mike; Salleo, Alberto; Ortmann, Frank; Mannsfeld, Stefan C.B.Self-assembled monolayers (SAMs) are widely employed in organic field-effect transistors to modify the surface energy, surface roughness, film growth kinetics, and electrical surface potential of the gate oxide to control the device's operating voltage. In this study, amino-functionalized SAM molecules are compared to pure alkylsilane SAMS in terms of their impact on the electrical properties of organic field-effect transistors, using the n-type polycrystalline small molecule semiconductor material N,N′-dioctyl-3,4,9,10-perylenedicarboximide (PTCDI-C8). In order to understand the electronic impact of the amino groups, the effect of both the number of amino-containing functional groups and the SAM molecular length are systematically studied. Though amino-functionalized SAM materials have been studied previously, this study is, for the first time, able to shed light on the nature of the doping effect that occurs when the gate oxide is treated with polar aminosilane materials. By a comprehensive theoretical study of the interface on the molecular level, it is shown that the observed shift in the threshold voltage is caused by free charges, which are attracted to the PTCDI-C8 and are stabilized there by protonated aminosilanes. This attraction and the voltage shift can be systematically tuned by varying the length of the neutral terminal chain of the aminosilane. © 2021 The Authors. Advanced Materials Interfaces published by Wiley-VCH GmbH
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