A novel strategy for efficient growth of nitrogen-doped graphene (N-graphene) on a large scale from s-triazine molecules is presented. The growth process has been unveiled in situ using ...time-dependent photoemission. It has been established that a postannealing of N-graphene after gold intercalation causes a conversion of the N environment from pyridinic to graphitic, allowing to obtain more than 80% of all embedded nitrogen in graphitic form, which is essential for the electron doping in graphene. A band gap, a doping level of 300 meV, and a charge-carrier concentration of ∼8 × 1012 electrons per cm2, induced by 0.4 atom % of graphitic nitrogen, have been detected by angle-resolved photoemission spectroscopy, which offers great promise for implementation of this system in next generation electronic devices.
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.
We show by angle-resolved photoemission spectroscopy that a tunable gap in quasi-free-standing monolayer graphene on Au can be induced by hydrogenation. The size of the gap can be controlled via ...hydrogen loading and reaches ∼1.0 eV for a hydrogen coverage of 8%. The local rehybridization from sp2 to sp3 in the chemical bonding is observed by X-ray photoelectron spectroscopy and X-ray absorption and allows for a determination of the amount of chemisorbed hydrogen. The hydrogen induced gap formation is completely reversible by annealing without damaging the graphene. Calculations of the hydrogen loading dependent core level binding energies and the spectral function of graphene are in excellent agreement with photoemission experiments. Hydrogenation of graphene gives access to tunable electronic and optical properties and thereby provides a model system to study hydrogen storage in carbon materials.
The hybridization between localized 4f electrons and itinerant electrons in rare-earth-based materials gives rise to their exotic properties like valence fluctuations, Kondo behaviour, ...heavy-fermions, or unconventional superconductivity. Here we present an angle-resolved photoemission spectroscopy (ARPES) study of the Kondo lattice antiferromagnet CeRh2Si2, where the surface and bulk Ce-4f spectral responses were clearly resolved. The pronounced 4f (0) peak seen for the Ce terminated surface gets strongly suppressed in the bulk Ce-4f spectra taken from a Si-terminated crystal due to much larger f-d hybridization. Most interestingly, the bulk Ce-4f spectra reveal a fine structure near the Fermi edge reflecting the crystal electric field splitting of the bulk magnetic 4f (1)5/2 state. This structure presents a clear dispersion upon crossing valence states, providing direct evidence of f-d hybridization. Our findings give precise insight into f-d hybridization penomena and highlight their importance in the antiferromagnetic phases of Kondo lattices.
Electron-phonon coupling and the emergence of superconductivity in intercalated graphite have been studied extensively. Yet, phonon-mediated superconductivity has never been observed in the 2D ...equivalent of these materials, doped monolayer graphene. Here we perform angle-resolved photoemission spectroscopy to try to find an electron donor for graphene that is capable of inducing strong electron-phonon coupling and superconductivity. We examine the electron donor species Cs, Rb, K, Na, Li, Ca and for each we determine the full electronic band structure, the Eliashberg function and the superconducting critical temperature Tc from the spectral function. An unexpected low-energy peak appears for all dopants with an energy and intensity that depend on the dopant atom. We show that this peak is the result of a dopant-related vibration. The low energy and high intensity of this peak are crucially important for achieving superconductivity, with Ca being the most promising candidate for realizing superconductivity in graphene.
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.
Sponges are probably the earliest branching animals, and their fossil record dates back to the Precambrian. Identifying their skeletal structure and composition is thus a crucial step in improving ...our understanding of the early evolution of metazoans. Here, we present the discovery of 505-million-year-old chitin, found in exceptionally well preserved Vauxia gracilenta sponges from the Middle Cambrian Burgess Shale. Our new findings indicate that, given the right fossilization conditions, chitin is stable for much longer than previously suspected. The preservation of chitin in these fossils opens new avenues for research into other ancient fossil groups.
Discovered in 1962, the divalent ferromagnetic semiconductor EuS (T C = 16.5 K, E g = 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 T C 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 T C 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.
The Kondo model predicts that both the valence at low temperatures and its temperature dependence scale with the characteristic energy T
of the Kondo interaction. Here, we study the evolution of the ...4f occupancy with temperature in a series of Yb Kondo lattices using resonant X-ray emission spectroscopy. In agreement with simple theoretical models, we observe a scaling between the valence at low temperature and T
obtained from thermodynamic measurements. In contrast, the temperature scale T
at which the valence increases with temperature is almost the same in all investigated materials while the Kondo temperatures differ by almost four orders of magnitude. This observation is in remarkable contradiction to both naive expectation and precise theoretical predictions of the Kondo model, asking for further theoretical work in order to explain our findings. Our data exclude the presence of a quantum critical valence transition in YbRh
Si
.
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.
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