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The discovery of a square magnetic-skyrmion lattice in GdRu2Si2, with the smallest so far found skyrmion size and without a geometrically frustrated lattice, has attracted significant attention. In this work, we present a comprehensive study of surface and bulk electronic structures of GdRu2Si2 by utilizing momentum-resolved photoemission (ARPES) measurements and first-principles calculations. We show how the electronic structure evolves during the antiferromagnetic transition when a peculiar helical order of 4f magnetic moments within the Gd layers sets in. A nice agreement of the ARPES-derived electronic structure with the calculated one has allowed us to characterize the features of the Fermi surface (FS), unveil the nested region along kz at the corner of the 3D FS, and reveal their orbital compositions. Our findings suggest that the Ruderman-Kittel-Kasuya-Yosida interaction plays a decisive role in stabilizing the spiral-like order of Gd 4f moments responsible for the skyrmion physics in GdRu2Si2. Our results provide a deeper understanding of electronic and magnetic properties of this material, which is crucial for predicting and developing novel skyrmion-based systems.
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Collective spin excitations in magnetically ordered crystals, called magnons or spin waves, can serve as carriers in novel spintronic devices with ultralow energy consumption. The generation of well-detectable spin flows requires long lifetimes of high-frequency magnons. In general, the lifetime of spin waves in a metal is substantially reduced due to a strong coupling of magnons to the Stoner continuum. This makes metals unattractive for use as components for magnonic devices. Here, we present the metallic antiferromagnet CeCo2P2, which exhibits long-living magnons even in the terahertz (THz) regime. For CeCo2P2, our first-principle calculations predict a suppression of low-energy spin-flip Stoner excitations, which is verified by resonant inelastic X-ray scattering measurements. By comparison to the isostructural compound LaCo2P2, we show how small structural changes can dramatically alter the electronic structure around the Fermi level leading to the classical picture of the strongly damped magnons intrinsic to metallic systems. Our results not only demonstrate that long-lived magnons in the THz regime can exist in bulk metallic systems, but they also open a path for an efficient search for metallic magnetic systems in which undamped THz magnons can be excited.
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The orientation of the 4f moments offers an additional degree of freedom for engineering the spin-related properties in spintronic nanostructures of lanthanides. Yet, precise monitoring of the direction of magnetic moments remains a challenge. Here, on the example of the antiferromagnets HoRh2Si2 and DyRh2Si2, we investigate the temperature-dependent canting of the 4f moments near the surface. We demonstrate that this canting can be understood in the framework of crystal electric field theory and the exchange magnetic interaction. Using photoelectron spectroscopy, we disclose subtle but certain temperature-dependent changes in the line shape of the 4f multiplet. These changes are directly linked to the canting of the 4f moments, which is different for the individual lanthanide layers near the surface. Our results illustrate the opportunity to monitor the orientation of the 4f-moments with high precision, which is essential for development of novel lanthanide-based nanostructures, interfaces, supramolecular complexes, and single-molecule magnets for various applications.
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The nature of the antiferromagnetic order in the heavy fermion metal YbRh_{2}Si_{2}, its quantum criticality, and superconductivity, which appears at low mK temperatures, remain open questions. We report measurements of the heat capacity over the wide temperature range 180 µK-80 mK, using current sensing noise thermometry. In zero magnetic field we observe a remarkably sharp heat capacity anomaly at 1.5 mK, which we identify as an electronuclear transition into a state with spatially modulated electronic magnetic order of maximum amplitude 0.1 µ_{B}. We also report results of measurements in magnetic fields in the range 0 to 70 mT, applied perpendicular to the c axis, which show eventual suppression of this order. These results demonstrate a coexistence of a large moment antiferromagnet with putative superconductivity.
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Ultrafast manipulation of magnetism bears great potential for future information technologies. While demagnetization in ferromagnets is governed by the dissipation of angular momentum1-3, materials with multiple spin sublattices, for example antiferromagnets, can allow direct angular momentum transfer between opposing spins, promising faster functionality. In lanthanides, 4f magnetic exchange is mediated indirectly through the conduction electrons4 (the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction), and the effect of such conditions on direct spin transfer processes is largely unexplored. Here, we investigate ultrafast magnetization dynamics in 4f antiferromagnets and systematically vary the 4f occupation, thereby altering the magnitude of the RKKY coupling energy. By combining time-resolved soft X-ray diffraction with ab initio calculations, we find that the rate of direct transfer between opposing moments is directly determined by this coupling. Given the high sensitivity of RKKY to the conduction electrons, our results offer a useful approach for fine tuning the speed of magnetic devices.
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Discovered in 1962, the divalent ferromagnetic semiconductor EuS (TC = 16.5 K, Eg = 1.65 eV) has remained constantly relevant to the engineering of novel magnetically active interfaces, heterostructures, and multilayer sequences and to combination with topological materials. Because detailed information on the electronic structure of EuS and, in particular, its evolution across TC is not well-represented in the literature but is essential for the development of new functional systems, the present work aims at filling this gap. Our angle-resolved photoemission measurements complemented with first-principles calculations demonstrate how the electronic structure of EuS evolves across a paramagnetic-ferromagnetic transition. Our results emphasize the importance of the strong Eu 4f-S 3p mixing for exchange-magnetic splittings of the sulfur-derived bands as well as coupling between f and d orbitals of neighboring Eu atoms to derive the value of TC accurately. The 4f-3p mixing facilitates the coupling between 4f and 5d orbitals of neighboring Eu atoms, which mainly governs the exchange interaction in EuS.
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The heavy-fermion behavior in intermetallic compounds manifests itself in a quenching of local magnetic moments by developing Kondo spin-singlet many-body states combined with a drastic increase of the effective mass of conduction electrons, which occurs below the lattice Kondo temperatureTK. This behavior is caused by interactions between the strongly localized 4felectrons and itinerant electrons. A controversially discussed question in this context is how the localized electronic states contribute to the Fermi surface upon changing the temperature. One expects that hybridization between the local moments and the itinerant electrons leads to a transition from a small Fermi surface in a non-coherent regime at high temperatures to a large Fermi surface once the coherent Kondo lattice regime is realized belowTK. We demonstrate, using hard x-ray angle-resolved photoemission spectroscopy that the electronic structure of the prototypical heavy fermion compound YbRh2Si2changes with temperature between 100 and 200 K, i.e. far above the Kondo temperature,TK= 25 K, of this system. Our results suggest a transition from a small to a large Fermi surface with decreasing temperature. This result is inconsistent with the prediction of the dynamical mean-field periodic Anderson model and supports the idea of an independent energy scale governing the change of band dispersion.
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The magnetocrystalline anisotropy of GdRh2Si2 is examined in detail via the electron spin resonance (ESR) of its well-localised Gd3+ moments. Below T N = 107 K, long range magnetic order sets in with ferromagnetic layers in the (aa)-plane stacked antiferromagnetically along the c-axis of the tetragonal structure. Interestingly, the easy-plane anisotropy allows for the observation of antiferromagnetic resonance at X- and Q-band microwave frequencies. In addition to the easy-plane anisotropy we have also quantified the weaker fourfold anisotropy within the easy plane. The obtained resonance fields are modelled in terms of eigenoscillations of the two antiferromagnetically coupled sublattices. Conversely, this model provides plots of the eigenfrequencies as a function of field and the specific anisotropy constants. Such calculations have rarely been done. Therefore our analysis is prototypical for other systems with fourfold in-plane anisotropy. It is demonstrated that the experimental in-plane ESR data may be crucial for a precise knowledge of the out-of-plane anisotropy.
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Spin-orbit interaction and structure inversion asymmetry in combination with magnetic ordering is a promising route to novel materials with highly mobile spin-polarized carriers at the surface. Spin-resolved measurements of the photoemission current from the Si-terminated surface of the antiferromagnet TbRh_{2}Si_{2} and their analysis within an ab initio one-step theory unveil an unusual triple winding of the electron spin along the fourfold-symmetric constant energy contours of the surface states. A two-band k·p model is presented that yields the triple winding as a cubic Rashba effect. The curious in-plane spin-momentum locking is remarkably robust and remains intact across a paramagnetic-antiferromagnetic transition in spite of spin-orbit interaction on Rh atoms being considerably weaker than the out-of-plane exchange field due to the Tb 4f moments.
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Single crystals of HoIr2Si2 with the body-centered ThCr2Si2-type structure (I4/mmm) were grown by Bridgman method from indium flux. Single crystal structure determination yielded a Si-z position of 0.378(1) in the structure. We excluded the presence of the high temperature phase with the primitive CaBe2Ge2-type structure (P4/nmm) by powder x-ray diffraction. Magnetic measurements on the single crystals yield a Néel temperature of [Formula: see text] K. In the inverse magnetic susceptibility a strong anisotropy with Weiss temperatures [Formula: see text] K and [Formula: see text] K occurs above T N. The effective magnetic moment [Formula: see text] and [Formula: see text] is close to the expected value for a free Ho3+ ion, [Formula: see text]. The field dependent magnetization shows a step-like behaviour due to crystalline electric field effects. The temperature and field dependence of the magnetization hint to the ordering of the magnetic moments along the c direction below T N.
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A ferromagnetic quantum critical point is thought not to exist in two- and three-dimensional metallic systems yet is realized in the Kondo lattice compound YbNi_{4}(P,As)_{2}, possibly due to its one-dimensionality. It is crucial to investigate the dimensionality of the Fermi surface of YbNi_{4}P_{2} experimentally, but common probes such as angle-resolved photoemission spectroscopy and quantum oscillation measurements are lacking. Here, we study the magnetic-field dependence of transport and thermodynamic properties of YbNi_{4}P_{2}. The Kondo effect is continuously suppressed, and additionally we identify nine Lifshitz transitions between 0.4 and 18 T. We analyze the transport coefficients in detail and identify the type of Lifshitz transitions as neck or void type to gain information on the Fermi surface of YbNi_{4}P_{2}. The large number of Lifshitz transitions observed within this small energy window is unprecedented and results from the particular flat renormalized band structure with strong 4f-electron character shaped by the Kondo lattice effect.
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Spin-polarized two-dimensional electron states (2DESs) at surfaces and interfaces of magnetically active materials attract immense interest because of the idea of exploiting fermion spins rather than charge in next generation electronics. Applying angle-resolved photoelectron spectroscopy, we show that the silicon surface of GdRh2Si2 bears two distinct 2DESs, one being a Shockley surface state, and the other a Dirac surface resonance. Both are subject to strong exchange interaction with the ordered 4f-moments lying underneath the Si-Rh-Si trilayer. The spin degeneracy of the Shockley state breaks down below ~90 K, and the splitting of the resulting subbands saturates upon cooling at values as high as ~185 meV. The spin splitting of the Dirac state becomes clearly visible around ~60 K, reaching a maximum of ~70 meV. An abrupt increase of surface magnetization at around the same temperature suggests that the Dirac state contributes significantly to the magnetic properties at the Si surface. We also show the possibility to tune the properties of 2DESs by depositing alkali metal atoms. The unique temperature-dependent ferromagnetic properties of the Si-terminated surface in GdRh2Si2 could be exploited when combined with functional adlayers deposited on top for which novel phenomena related to magnetism can be anticipated.