Abstract
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 CeCo
2
P
2
, which exhibits long-living magnons even in the terahertz (THz) regime. For CeCo
2
P
2
, 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 LaCo
2
P
2
, 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.
The magnetocrystalline anisotropy of GdRh2Si2 is examined in detail via the electron spin resonance (ESR) of its well-localised Gd3+ moments. Below TN = 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.
Many tetragonal compounds LnIr2Si2 (Ln = lanthanoid) occur in two polymorphous phases and are therefore well suited to study the relationship between crystal structure and magnetic properties. We ...have grown GdIr2Si2 single crystals of both polymorphs from a high-temperature indium flux and investigated their anisotropic magnetic properties. The higher symmetric form with the ThCr2Si2 structure (space group I4/mmm) orders antiferromagnetically at TN=87K while for the lower symmetric compound in the CaBe2Ge2 structure (space group P4/nmm) we determined a much lower Néel temperature TN=12K. Our magnetic characterization of the single crystals reveals that for both compounds the magnetic moments are aligned in the a−a plane of the tetragonal lattice, but that the change of the symmetry strongly effects the inplane alignment of the moment orientation. For Ln=Er and Ho, we confirmed the existence of LnIr2Si2 in the space group P4/nmm. The magnetic properties of these lower symmetric compounds are in remarkable difference to their related compounds in the space group I4/mmm.
•Successful single crystal growth of two polymorphous phases of GdIr2Si2.•Observation of very different magnetic properties for the two phases of GdIr2Si2.•Characterization and comparison of related polymorphism in HoIr2Si2 and ErIr2Si2.
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 K. In the inverse magnetic susceptibility a strong anisotropy with Weiss temperatures K and K occurs above TN. The effective magnetic moment and is close to the expected value for a free Ho3+ ion, . 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 TN.
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 TbRh2Si2 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 4 f moments.
Ultrafast manipulation of magnetism bears great potential for future information technologies. While demagnetization in ferromagnets is governed by the dissipation of angular momentum
, 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 electrons
(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.
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.
One of the most successful paradigms of many-body physics is the concept of quasiparticles: excitations in strongly interacting matter behaving like weakly interacting particles in free space. ...Quasiparticles in metals are very robust objects. Nevertheless, when a system’s ground state undergoes a qualitative change at a quantum critical point (QCP)1, the quasiparticles may disintegrate and give way to an exotic quantum-fluid state of matter. The nature of this breakdown is intensely debated2–5, because the emergent quantum fluid dominates material properties up to high temperatures and might even be related to the occurrence of superconductivity in some compounds6. Here we trace the dynamics of heavy-fermion quasiparticles in CeCu6−xAux and monitor their evolution towards the QCP in time-resolved experiments, supported by many-body calculations. A terahertz pulse disrupts the many-body heavy-fermion state. Under emission of a delayed, phase-coherent terahertz reflex the heavy-fermion state recovers, with a coherence time 100 times longer than typically associated with correlated metals7,8. The quasiparticle weight collapses towards the QCP, yet its formation temperature remains constant—phenomena believed to be mutually exclusive. Coexistence in the same experiment calls for revisions in our view on quantum criticality.
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