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- ItemStripe-yzmagnetic order in the triangular-lattice antiferromagnet KCeS2(Bristol : IOP Publ., 2021) Kulbakov, Anton A.; Avdoshenko, Stanislav M.; Puente-Orench, Inés; Deeb, Mahmoud; Doerr, Mathias; Schlender, Philipp; Doert, Thomas; Inosov, Dmytro S.Yb- and Ce-based delafossites were recently identified as effective spin-1/2 antiferromagnets on the triangular lattice. Several Yb-based systems, such as NaYbO2, NaYbS2, and NaYbSe2, exhibit no long-range order down to the lowest measured temperatures and therefore serve as putative candidates for the realization of a quantum spin liquid. However, their isostructural Ce-based counterpart KCeS2 exhibits magnetic order below TN = 400 mK, which was so far identified only in thermodynamic measurements. Here we reveal the magnetic structure of this long-range ordered phase using magnetic neutron diffraction. We show that it represents the so-called 'stripe-yz' type of antiferromagnetic order with spins lying approximately in the triangular-lattice planes orthogonal to the nearest-neighbor Ce–Ce bonds. No structural lattice distortions are revealed below TN, indicating that the triangular lattice of Ce3+ ions remains geometrically perfect down to the lowest temperatures. We propose an effective Hamiltonian for KCeS2, based on a fit to the results of ab initio calculations, and demonstrate that its magnetic ground state matches the experimental spin structure.
- ItemThe Weak 3D Topological Insulator Bi12Rh3Sn3I9(Weinheim : Wiley-VCH, 2020) Lê Anh, Mai; Kaiser, Martin; Ghimire, Madhav Prasad; Richter, Manuel; Koepernik, Klaus; Gruschwitz, Markus; Tegenkamp, Christoph; Doert, Thomas; Ruck, MichaelTopological insulators (TIs) gained high interest due to their protected electronic surface states that allow dissipation-free electron and information transport. In consequence, TIs are recommended as materials for spintronics and quantum computing. Yet, the number of well-characterized TIs is rather limited. To contribute to this field of research, we focused on new bismuth-based subiodides and recently succeeded in synthesizing a new compound Bi12Rh3Sn3I9, which is structurally closely related to Bi14Rh3I9 – a stable, layered material. In fact, Bi14Rh3I9 is the first experimentally supported weak 3D TI. Both structures are composed of well-defined intermetallic layers of ∞2[(Bi4Rh)3I]2+ with topologically protected electronic edge-states. The fundamental difference between Bi14Rh3I9 and Bi12Rh3Sn3I9 lies in the composition and the arrangement of the anionic spacer. While the intermetallic 2D TI layers in Bi14Rh3I9 are isolated by ∞1[Bi2I8]2− chains, the isoelectronic substitution of bismuth(III) with tin(II) leads to ∞2[Sn3I8]2− layers as anionic spacers. First transport experiments support the 2D character of this material class and revealed metallic conductivity. © 2020 The Authors. Published by Wiley-VCH GmbH
- ItemLong-range magnetic order in the ~S=1/2 triangular lattice antiferromagnet KCeS2(Amsterdam : SciPost Foundation, 2020) Bastien, Gaël; Rubrecht, Bastian; Haeussler, Ellen; Schlender, Philipp; Zangeneh, Ziba; Avdoshenko, Stanislav; Sarkar, Rajib; Alfonsov, Alexey; Luther, Sven; Onykiienko, Yevhen A.; Walker, Helen C.; Kühne, Hannes; Grinenko, Vadim; Guguchia, Zurab; Kataev, Vladislav; Klauss, Hans-Henning; Hozoi, Liviu; van den Brink, Jeroen; Inosov, Dmytro S.; Büchner, Bernd; Wolter, Anja U.B.; Doert, ThomasRecently, several putative quantum spin liquid (QSL) states were discovered in ~S=1/2 rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. A way to clarify the origin of the QSL state in these systems is to identify ways to tune them from the putative QSL state towards long-range magnetic order. Here, we introduce the Ce-based TLAF KCeS2 and show via low-temperature specific heat and μSR investigations that it yields magnetic order below TN=0.38 K despite the same delafossite structure. We identify a well separated ~S=1/2 ground state for KCeS2 from inelastic neutron scattering and embedded-cluster quantum chemical calculations. Magnetization and electron spin resonance measurements on single crystals indicate a strong easy-plane g~factor anisotropy, in agreement with the ab initio calculations. Finally, our specific-heat studies reveal an in-plane anisotropy of the magnetic field-temperature phase diagram which may indicate anisotropic magnetic interactions in KCeS2.
- ItemFreestanding few-layer sheets of a dual topological insulator(London : Nature Publishing Group, 2021) Anh, Mai Lê; Potapov, Pavel; Lubk, Axel; Doert, Thomas; Ruck, MichaelThe emergence of topological insulators (TIs) raised high expectations for their application in quantum computers and spintronics. Being bulk semiconductors, their nontrivial topology at the electronic bandgap enables dissipation-free charge and spin transport in protected metallic surface states. For application, crystalline thin films are requested in sufficient quantity. A suitable approach is the liquid phase exfoliation (LPE) of TI crystals that have layered structures. Bi2TeI is a weak 3D TI, which leads to protected edge states at the side facets of a crystal, as well as a topological crystalline insulator, which is responsible for protected states at the top and bottom faces. We developed an effective, scalable protocol for LPE of freestanding nanoflakes from Bi2TeI crystals. By heat treatment and sonication in isopropyl alcohol and poly(vinylpyrrolidone), crystalline Bi2TeI sheets with a thickness of ~50 nm were obtained and can therefore be considered for further processing toward microelectronic applications.
- ItemFreestanding Nanolayers of a Wide-Gap Topological Insulator through Liquid-Phase Exfoliation(Weinheim : Wiley-VCH, 2021) Lê Anh, Mai; Potapov, Pavel; Wolf, Daniel; Lubk, Axel; Glatz, Bernhard; Fery, Andreas; Doert, Thomas; Ruck, MichaelThe layered salt Bi14Rh3I9 is a weak three-dimensional (3D) topological insulator (TI), that is, a stack of two-dimensional (2D) TIs. It has a wide non-trivial band gap of 210 meV, which is generated by strong spin-orbit coupling, and possesses protected electronic edge-states. In the structure, charged layers of (Formula presented.) (Bi4Rh)3I]2+ honeycombs and (Formula presented.) Bi2I8]2− chains alternate. The non-trivial topology of Bi14Rh3I9 is an inherent property of the 2D intermetallic fragment. Here, the exfoliation of Bi14Rh3I9 was performed using two different chemical approaches: (a) through a reaction with n-butyllithium and poly(vinylpyrrolidone), (b) through a reaction with betaine in dimethylformamide at 55 °C. The former yielded few-layer sheets of the new compound Bi12Rh3I, while the latter led to crystalline sheets of Bi14Rh3I9 with a thickness down to 5 nm and edge-lengths up to several ten microns. X-ray diffraction and electron microscopy proved that the structure of Bi14Rh3I9 remained intact. Thus, it was assumed that the particles are still TIs. Dispersions of these flakes now allow for next steps towards the envisioned applications in nanoelectronics, such as the study of quantum coherence in deposited films, the combination with superconducting particles or films for the generation of Majorana fermions, or studies on their behavior under the influence of magnetic or electric fields or in contact with various materials occurring in devices. The method presented generally allows to exfoliate layers with high specific charges and thus the use of layered starting materials beyond van der Waals crystals. © 2020 The Authors. Chemistry - A European Journal published by Wiley-VCH GmbH
- ItemMechanism of Bi−Ni Phase Formation in a Microwave-Assisted Polyol Process(Weinheim : Wiley-VCH, 2019) Smuda, Matthias; Damm, Christine; Ruck, Michael; Doert, ThomasTypically, intermetallic phases are obtained in solid-state reactions or crystallization from melts, which are highly energy and time consuming. The polyol process takes advantage of low temperatures and short reaction times using easily obtainable starting materials. The formation mechanism of these intermetallic particles has received little attention so far, even though a deeper understanding should allow for better synthesis planning. In this study, we therefore investigated the formation of BiNi particles in ethylene glycol in a microwave-assisted polyol process mechanistically. The coordination behavior in solution was analyzed using HPLC-MS and UV-Vis. Tracking the reaction with PXRD measurements, FT-IR spectroscopy and HR-TEM revealed a successive reduction of Bi3+ and Ni2+, leading to novel spherical core-shell structure in a first reaction step. Bismuth particles are encased in a matrix of nickel nanoparticles of 2 nm to 6 nm in diameter and oxidation products of ethylene glycol. Step-wise diffusion of nickel into the bismuth particle intermediately results in the bismuth-rich compound Bi3Ni, which consecutively transforms into the BiNi phase as the reaction progresses. The impacts of the anion type, temperature and pH value were also investigated. © 2020 The Authors. Published by Wiley-VCH GmbH