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In Situ Fabrication of Freestanding Single-Atom-Thick 2D Metal/Metallene and 2D Metal/ Metallene Oxide Membranes: Recent Developments

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.

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Imaging and writing magnetic domains in the non-collinear antiferromagnet Mn3Sn

2019, Reichlova, Helena, Janda, Tomas, Godinho, Joao, Markou, Anastasios, Kriegner, Dominik, Schlitz, Richard, Zelezny, Jakub, Soban, Zbynek, Bejarano, Mauricio, Schultheiss, Helmut, Nemec, Petr, Jungwirth, Tomas, Felser, Claudia, Wunderlich, Joerg, Goennenwein, Sebastian T. B.

Non-collinear antiferromagnets are revealing many unexpected phenomena and they became crucial for the field of antiferromagnetic spintronics. To visualize and prepare a well-defined domain structure is of key importance. The spatial magnetic contrast, however, remains extraordinarily difficult to be observed experimentally. Here, we demonstrate a magnetic imaging technique based on a laser induced local thermal gradient combined with detection of the anomalous Nernst effect. We employ this method in one the most actively studied representatives of this class of materials—Mn3Sn. We demonstrate that the observed contrast is of magnetic origin. We further show an algorithm to prepare a well-defined domain pattern at room temperature based on heat assisted recording principle. Our study opens up a prospect to study spintronics phenomena in non-collinear antiferromagnets with spatial resolution.

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Retrieving spin textures on curved magnetic thin films with full-field soft X-ray microscopies

2015, Streubel, Robert, Kronast, Florian, Fischer, Peter, Parkinson, Dula, Schmidt, Oliver G., Makarov, Denys

X-ray tomography is a well-established technique to characterize 3D structures in material sciences and biology; its magnetic analogue--magnetic X-ray tomography--is yet to be developed. Here we demonstrate the visualization and reconstruction of magnetic domain structures in a 3D curved magnetic thin films with tubular shape by means of full-field soft X-ray microscopies. The 3D arrangement of the magnetization is retrieved from a set of 2D projections by analysing the evolution of the magnetic contrast with varying projection angle. Using reconstruction algorithms to analyse the angular evolution of 2D projections provides quantitative information about domain patterns and magnetic coupling phenomena between windings of azimuthally and radially magnetized tubular objects. The present approach represents a first milestone towards visualizing magnetization textures of 3D curved thin films with virtually arbitrary shape.

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Collapse of layer dimerization in the photo-induced hidden state of 1T-TaS2

2020, Stahl, Quirin, Kusch, Maximilian, Heinsch, Florian, Garbarino, Gaston, Kretzschmar, Norman, Hanff, Kerstin, Rossnagel, Kai, Geck, Jochen, Ritschel, Tobias

Photo-induced switching between collective quantum states of matter is a fascinating rising field with exciting opportunities for novel technologies. Presently, very intensively studied examples in this regard are nanometer-thick single crystals of the layered material 1T-TaS2, where picosecond laser pulses can trigger a fully reversible insulator-to-metal transition (IMT). This IMT is believed to be connected to the switching between metastable collective quantum states, but the microscopic nature of this so-called hidden quantum state remained largely elusive up to now. Here, we characterize the hidden quantum state of 1T-TaS2 by means of state-of-the-art x-ray diffraction and show that the laser-driven IMT involves a marked rearrangement of the charge and orbital order in the direction perpendicular to the TaS2-layers. More specifically, we identify the collapse of interlayer molecular orbital dimers as a key mechanism for this non-thermal collective transition between two truly long-range ordered electronic crystals.

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Electron beam induced dehydrogenation of MgH2 studied by VEELS

2016, Surrey, Alexander, Schultz, Ludwig, Rellinghaus, Bernd

Nanosized or nanoconfined hydrides are promising materials for solid-state hydrogen storage. Most of these hydrides, however, degrade fast during the structural characterization utilizing transmission electron microscopy (TEM) upon the irradiation with the imaging electron beam due to radiolysis. We use ball-milled MgH2 as a reference material for in-situ TEM experiments under low-dose conditions to study and quantitatively understand the electron beam-induced dehydrogenation. For this, valence electron energy loss spectroscopy (VEELS) measurements are conducted in a monochromated FEI Titan3 80–300 microscope. From observing the plasmonic absorptions it is found that MgH2 successively converts into Mg upon electron irradiation. The temporal evolution of the spectra is analyzed quantitatively to determine the thickness-dependent, characteristic electron doses for electron energies of both 80 and 300 keV. The measured electron doses can be quantitatively explained by the inelastic scattering of the incident high-energy electrons by the MgH2 plasmon. The obtained insights are also relevant for the TEM characterization of other hydrides.

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Tomonaga–Luttinger liquid behavior and spinon confinement in YbAlO 3

2019, Wu, L.S., Nikitin, S.E., Wang, Z., Zhu, W., Batista, C.D., Tsvelik, A.M., Samarakoon, A.M., Tennant, D.A., Brando, M., Vasylechko, L., Frontzek, M., Savici, A.T., Sala, G., Ehlers, G., Christianson, A.D., Lumsden, M.D., Podlesnyak, A.

Low dimensional quantum magnets are interesting because of the emerging collective behavior arising from strong quantum fluctuations. The one-dimensional (1D) S = 1/2 Heisenberg antiferromagnet is a paradigmatic example, whose low-energy excitations, known as spinons, carry fractional spin S = 1/2. These fractional modes can be reconfined by the application of a staggered magnetic field. Even though considerable progress has been made in the theoretical understanding of such magnets, experimental realizations of this low-dimensional physics are relatively rare. This is particularly true for rare-earth-based magnets because of the large effective spin anisotropy induced by the combination of strong spin–orbit coupling and crystal field splitting. Here, we demonstrate that the rare-earth perovskite YbAlO3 provides a realization of a quantum spin S = 1/2 chain material exhibiting both quantum critical Tomonaga–Luttinger liquid behavior and spinon confinement–deconfinement transitions in different regions of magnetic field–temperature phase diagram.

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Integrated molecular diode as 10 MHz half-wave rectifier based on an organic nanostructure heterojunction

2020, Li, Tianming, Bandari, Vineeth Kumar, Hantusch, Martin, Xin, Jianhui, Kuhrt, Robert, Ravishankar, Rachappa, Xu, Longqian, Zhang, Jidong, Knupfer, Martin, Zhu, Feng, Yan, Donghang, Schmidt, Oliver G.

Considerable efforts have been made to realize nanoscale diodes based on single molecules or molecular ensembles for implementing the concept of molecular electronics. However, so far, functional molecular diodes have only been demonstrated in the very low alternating current frequency regime, which is partially due to their extremely low conductance and the poor degree of device integration. Here, we report about fully integrated rectifiers with microtubular soft-contacts, which are based on a molecularly thin organic heterojunction and are able to convert alternating current with a frequency of up to 10 MHz. The unidirectional current behavior of our devices originates mainly from the intrinsically different surfaces of the bottom planar and top microtubular Au electrodes while the excellent high frequency response benefits from the charge accumulation in the phthalocyanine molecular heterojunction, which not only improves the charge injection but also increases the carrier density.

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Pressure-tuning the quantum spin Hamiltonian of the triangular lattice antiferromagnet Cs2CuCl4

2019, Zvyagin, S.A., Graf, D., Sakurai, T., Kimura, S., Nojiri, H., Wosnitza, J., Ohta, H., Ono, T., Tanaka, H.

Quantum triangular-lattice antiferromagnets are important prototype systems to investigate numerous phenomena of the geometrical frustration in condensed matter. Apart from highly unusual magnetic properties, they possess a rich phase diagram (ranging from an unfrustrated square lattice to a quantum spin liquid), yet to be confirmed experimentally. One major obstacle in this area of research is the lack of materials with appropriate (ideally tuned) magnetic parameters. Using Cs2CuCl4 as a model system, we demonstrate an alternative approach, where, instead of the chemical composition, the spin Hamiltonian is altered by hydrostatic pressure. The approach combines high-pressure electron spin resonance and r.f. susceptibility measurements, allowing us not only to quasi-continuously tune the exchange parameters, but also to accurately monitor them. Our experiments indicate a substantial increase of the exchange coupling ratio from 0.3 to 0.42 at a pressure of 1.8 GPa, revealing a number of emergent field-induced phases.

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General synthesis of 2D rare-earth oxide single crystals with tailorable facets

2021, Li, Linyang, Lu, Fangyun, Xiong, Wenqi, Ding, Yu, Lu, Yangyi, Xiao, Yao, Tong, Xin, Wang, Yao, Jia, Shuangfeng, Wang, Jianbo, Mendes, Rafael G., Rümmeli, Mark H., Yuan, Shengjun, Zeng, Mengqi, Fu, Lei

Two-dimensional (2D) rare-earth oxides (REOs) are a large family of materials with various intriguing applications and precise facet control is essential for investigating new properties in the 2D limit. However, a bottleneck remains with regard to obtaining their 2D single crystals with specific facets because of the intrinsic non-layered structure and disparate thermodynamic stability of different facets. Herein, for the first time, we achieve the synthesis of a wide variety of high-quality 2D REO single crystals with tailorable facets via designing a hard-soft-acid-base couple for controlling the 2D nucleation of the predetermined facets and adjusting the growth mode and direction of crystals. Also, the facet-related magnetic properties of 2D REO single crystals were revealed. Our approach provides a foundation for further exploring other facet-dependent properties and various applications of 2D REO, as well as inspiration for the precise growth of other non-layered 2D materials.

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Publisher Correction: Multiple fermion scattering in the weakly coupled spin-chain compound YbAlO3 (Nature Communications, (2021), 12, 1, (3599), 10.1038/s41467-021-23585-z)

2021, Nikitin, S.E., Nishimoto, S., Fan, Y., Wu, J., Wu, L.S., Sukhanov, A.S., Brando, M., Pavlovskii, N.S., Xu, J., Vasylechko, L., Yu, R., Podlesnyak, A.

[No abstract available]