The complex electronic properties of ZrTe5 have recently stimulated in-depth investigations that assigned this material to either a topological insulator or a 3D Dirac semimetal phase. Here we report a comprehensive experimental and theoretical study of both electronic and structural properties of ZrTe5, revealing that the bulk material is a strong topological insulator (STI). By means of angle-resolved photoelectron spectroscopy, we identify at the top of the valence band both a surface and a bulk state. The dispersion of these bands is well captured by ab initio calculations for the STI case, for the specific interlayer distance measured in our x-ray diffraction study. Furthermore, these findings are supported by scanning tunneling spectroscopy revealing the metallic character of the sample surface, thus confirming the strong topological nature of ZrTe5.The discovery of topological insulators (TIs), characterized by metallic spin-polarized surface states connecting the bulk valence and conduction bands [1], has stimulated the search for novel topological phases of matter [2][3][4][5][6]. ZrTe 5 has recently emerged as a challenging system with unique, albeit poorly understood, electronic properties [7][8][9][10][11][12][13][14][15][16][17]. Magneto-transport [11], magneto-infrared [13] and optical spectroscopy [14] studies describe ZrTe 5 in terms of a 3D Dirac semimetal. Theoretical calculations have predicted its bulk electronic properties to lie in proximity of a topological phase transition between a strong and a weak TI (STI and WTI, respectively), where only the former displays topologically protected surface states at the experimentally accessible (010) surface [10]. The monolayer is also computed to be a 2D TI [10] and scanning tunneling microscopy/spectroscopy (STM/STS) experiments suggest the existence of topologically protected states at step edges [18,19]. However, the unambiguous identification of the topological phase of ZrTe 5 is still lacking.In this Letter we report on the STI character of the bulk ZrTe 5 by combining ab initio calculations and multiple experimental techniques, at temperature both above and below the one of the resistivity peak, T * ∼ 160 K [7][8][9]15]. Angleresolved photoelectron spectroscopy (ARPES) experiments in the ultraviolet (UV) and soft x-ray (SX) energy ranges reveal the presence of two distinct states at the top of the valence band (VB). On the basis of photon energy dependent studies, we ascribe the origin of these two states to the bulk and crystal surface, respectively. We have performed ab initio calculations of the topological phase diagram of ZrTe 5 , as a function of the interlayer distance b/2. Our measured band dispersion is in agreement with the calculations and it is consistent with the STI case for b/2 = 7.23 ± 0.02Å. This value has been confirmed for our specimen by x-ray diffraction (XRD) measurements. Furthermore, the 3D Dirac semimetal phase is not protected by crystalline symmetries, and it manifests only for the specific b/2 = 7.35Å at the boundar...
liquid-nitrogen temperature [3] or single atoms exhibiting extremely long magnetic relaxation times. [4][5][6] In particular, systems based on late lanthanide family elements, like Dy and Tb, have been largely in focus, including single-molecule, [2,3] singleatom, [4,5] or single-chain magnets. [7,8] Adsorption of SMMs on surfaces allows to study individual molecular units, as well as to realize transport schemes essential for the implementation of SMMs in molecular-scale spintronics or quantum computing devices. [9][10][11][12][13][14][15][16][17] However the transition from bulk to surface-supported systems often goes along with a substantial change or even loss of SMM properties, that is, magnetic moment, magnetic anisotropy, or magnetization behavior. [18][19][20][21] On metallic surfaces, the interaction of the magnetic moments with the surface is rather strong, which is evidenced by the observation of the Kondo effect. [22,23] Thus, benchmark measurements during the last years demonstrating magnetic bistability of surface-adsorbed SMMs have been reported on substrates, where molecules are electronically weakly coupled to -TbPc 2 on HOPG, [24] on MgO/Ag(100) [25] and on graphene/SiC, [26] pushing the blocking temperature (T B ) limit up to 9 K. On the other hand, DySc 2 N@C 80 monolayers on Au(111) [27] recently showed a hysteresis opening at temperatures up to 10 K. In this sense, lanthanide ions encaged in C 80 molecules reportedly outperform most SMMs by their combination of chemical robustness with slow magnetic relaxation. [27][28][29][30][31] To further push the magnetic lifetime in the monolayer regime two important criteria have to be fulfilled: the first requirement is to synthesize SMM compounds showing intrinsically high T B in the bulk. The second requires implementation of the appropriate methods for molecular deposition on substrates, which provide sufficient decoupling of the SMM from the surface.In this work we provide experimental evidence on outstanding slow magnetic relaxation in Dy 2 @C 80 (CH 2 Ph) sub-monolayers on a graphene/Ir(111) surface. The Dy 2 @C 80 (CH 2 Ph) molecules deposited by the electrospray deposition method are organized into islands as shown by low-temperature scanning tunneling microscopy (STM) imaging. We explore their magnetic properties by means of X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements. The analysis of the magnetic relaxation behavior of Dy 2 @C 80 (CH 2 Ph) adsorbed on graphene/Ir(111) yields a Single-molecule magnets (SMMs) are among the most promising building blocks for future magnetic data storage or quantum computing applications, owing to magnetic bistability and long magnetic relaxation times. The practical device integration requires realization of 2D surface assemblies of SMMs, where each magnetic unit shows magnetic relaxation being sufficiently slow at application-relevant temperatures. Using X-ray absorption spectroscopy and X-ray magnetic circular dichroism, it is shown that sub-monolayers of Dy ...
Single-molecule magnets (SMMs) incorporate key properties that make them promising candidates for the emerging field of spintronics. The challenge to realize ordered SMM arrangements on surfaces and at the same time to preserve the magnetic properties upon interaction with the environment is a crucial point on the way to applications. Here we employ inelastic electron tunneling spectroscopy (IETS) to address the magnetic properties in single Fe4 complexes that are adsorbed in a highly ordered arrangement on graphene/Ir(111). We are able to substantially reduce the influence of both the tunneling tip and the adsorption environment on the Fe4 complex during the measurements by using appropriate tunneling parameters in combination with the flat-lying Fe4H derivative and a weakly interacting surface. This allows us to perform noninvasive IETS studies on these bulky molecules. From the measurements we identify intermultiplet spin transitions and determine the intramolecular magnetic exchange interaction constant on a large number of molecules. Although a considerable scattering of the exchange constant values is observed, the distribution maximum is located at a value that coincides with that of the bulk. Our findings confirm a retained molecular magnetism of the Fe4H complex at the local scale and evaluate the influence of the environment on the magnetic exchange interaction.
The electronic properties of graphene can be efficiently altered upon interaction with the underlying substrate resulting in a dramatic change of charge carrier behavior. Here, the evolution of the local electronic properties of epitaxial graphene on a metal upon the controlled formation of multilayers, which are produced by intercalation of atomic carbon in graphene/Ir(111), is investigated. Using scanning tunneling microscopy and Landau-level spectroscopy, it is shown that for a monolayer and bilayers with small-angle rotations, Landau levels are fully suppressed, indicating that the metal-graphene interaction is largely confined to the first graphene layer. Bilayers with large twist angles as well as twisted trilayers demonstrate a sequence of pronounced Landau levels characteristic for a free-standing graphene monolayer pointing toward an effective decoupling of the top layer from the metal substrate. These findings give evidence for the controlled preparation of epitaxial graphene multilayers with a different degree of decoupling, which represent an ideal platform for future electronic and spintronic applications.
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