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Under temperature or pressure tuning, tetragonal EuPd2Si2 is known to undergo a valence transition from nearly divalent to nearly trivalent Eu accompanied by a volume reduction. Albeit intensive work, its microscopic origin is still being discussed. Here, we investigate the mechanism of the valence transition under volume compression by ab initio density functional theory (DFT) calculations. Our analysis of the electronic and magnetic properties of EuPd2Si2 when approaching the valence transition shows an enhanced c-f hybridization between localized Eu 4f states and itinerant conduction states (Eu 5d, Pd 4d, and Si 3p) where an electronic charge redistribution takes place. We observe that the change in the electronic structure is intimately related to the volume reduction where Eu-Pd(Si) bond lengths shorten and, for the transition to happen, we trace the delicate balance between electronic bandwidth, crystal field splitting, Coulomb repulsion, Hund's coupling and spin-orbit coupling. In a next step we compare and benchmark our DFT results to surface-sensitive photoemission data in which the mixed-valent properties of EuPd2Si2 are reflected in a simultaneous observation of divalent and trivalent signals from the Eu 4f shell. The study serves as well to explore the limits of density functional theory and the choice of exchange correlation functionals to describe such a phenomenon as a valence transition.
The maximum recoverable strain of most crystalline solids is less than 1% because plastic deformation or fracture usually occurs at a small strain. In this work, we show that a SrNi2P2 micropillar exhibits pseudoelasticity with a large maximum recoverable strain of ~14% under uniaxial compression via unique reversible structural transformation, double lattice collapse-expansion that is repeatable under cyclic loading. Its high yield strength (~3.8±0.5 GPa) and large maximum recoverable strain bring out the ultrahigh modulus of resilience (~146±19MJ/m3) a few orders of magnitude higher than that of most engineering materials. The double lattice collapse-expansion mechanism shows stress-strain behaviors similar with that of conventional shape memory alloys, such as hysteresis and thermo-mechanical actuation, even though the structural changes involved are completely different. Our work suggests that the discovery of a new class of high performance ThCr2Si2-structured materials will open new research opportunities in the field of pseudoelasticity
We demonstrate ultra-sharp (≲10 nm) lateral p-n junctions in graphene using electronic transport, scanning tunneling microscopy, and first principles calculations. The p-n junction lies at the boundary between differentially-doped regions of a graphene sheet, where one side is intrinsic and the other is charge-doped by proximity to a flake of α-RuCl3 across a thin insulating barrier. We extract the p-n junction contribution to the device resistance to place bounds on the junction width. We achieve an ultra-sharp junction when the boundary between the intrinsic and doped regions is defined by a cleaved crystalline edge of α-RuCl3 located 2 nm from the graphene. Scanning tunneling spectroscopy in heterostructures of graphene, hexagonal boron nitride, and α-RuCl3 shows potential variations on a sub-10 nm length scale. First principles calculations reveal the charge-doping of graphene decays sharply over just nanometers from the edge of the α-RuCl3 flake.
In the novel stoichiometric iron-based material RbEuFe4As4 superconductivity coexists with a peculiar long-range magnetic order of Eu 4f states; their coexistance is puzzling and represents a challenge for both experiment and theory. Using angle-resolved photoemission spectroscopy, resonant photoemission spectroscopy, Andreev reflection spectroscopy and scanning tunneling spectroscopy we have addressed this puzzle and unambigously shown that Fe- and Eu-derived states are largely decoupled and that superconducting and a long range magnetic orders exist almost independently from each other.
Continued advances in quantum technologies rely on producing nanometer-scale wires. Although several state-of-the-art nanolithographic technologies and bottom-up synthesis processes have been used to engineer these wires, critical challenges remain in growing uniform atomic-scale crystalline wires and constructing their network structures. Here, we discover a simple method to fabricate atomic-scale wires with various arrangements, including stripes, X-junctions, Y-junctions, and nanorings. Single-crystalline atomic-scale wires of a Mott insulator, whose bandgap is comparable to those of wide-gap semiconductors, are spontaneously grown on graphite substrates by pulsed-laser deposition. These wires are one unit cell thick and have an exact width of two and four unit cells (1.4 and 2.8 nm) and lengths up to a few micrometers. We show that the nonequilibrium reaction-diffusion processes may play an essential role in atomic pattern formation. Our findings offer a previously unknown perspective on the nonequilibrium self-organization phenomena on an atomic scale, paving a unique way for the quantum architecture of nano-network.
We present results of hard X-ray angle-resolved photoemission spectroscopy and photoemission diffraction measurements performed on high-quality single crystals of the valence transition compound EuPd2Si2 for temperatures 25~K ≤ T ≤ 300~K. At low temperatures we observe a Eu 4f valence v=2.5, % occupation number n=6.5, which decreases to v=2.1 for temperatures above the valence transition around TV≈160~K. The experimental valence numbers resulting from an evaluation of the Eu(III)/Eu(II) 3d core levels, are used for calculating band structures using density functional theory. The valence transition significantly changes the band structure as determined by angle-resolved photoemission spectroscopy. In particular, the Eu 5d valence bands are shifted to lower binding energies with increasing Eu 4f occupancy. To a lesser extent, bands derived from the Si 3p and Pd 4d orbitals are also affected. This observation suggests a partial charge transfer between Eu and Pd/Si sites. Comparison with {\it ab-initio} theory shows a good agreement with experiment, in particular concerning the unequal band shift with increasing Eu 4f occupancy.
The discovery of the 1144-phase, e.g. CaKFe4As4, creates opportunities to build novel intermetallics with alternative stacking of two parent compounds. Here we formalize the idea by defining a class of bulk crystalline solids with A-B stacking (including 1144-phases and beyond), which is a generalization of hetero-structures from few-layer or thin-film semi-conductors to bulk intermetallics. Theoretically, four families of phosphides \textit{AB}(TM)4P4 (TM=Fe, Ru, Co, Ni) are investigated by first-principles calculations, wherein configurational, vibrational and electronic degrees of freedom are considered. It predicts a variety of stable 1144-phases (especially Ru- and Fe-phosphides). Stability rules are found and structural/electronic properties are discussed. Experimentally, we synthesize high-purity CaKRu4P4 as a proof of principle example. The synthetic method is simple and easily applied. Moreover, it alludes to a strategy to explore complex multi-component compounds, facilitated by a phase diagram coordinated by collective descriptors.
Rich functionalities of transition-metal oxides and their interfaces bear an enormous technological potential. Its realization in practical devices requires, however, a significant improvement of yet relatively low electron mobility in oxide materials. Recently, a mobility boost of about two orders of magnitude has been demonstrated at the spinel/perovskite {\gamma}-Al2O3/SrTiO3 interface compared to the paradigm perovskite/perovskite LaAlO3/SrTiO3. We explore the fundamental physics behind this phenomenon from direct measurements of the momentum-resolved electronic structure of this interface using resonant soft-X-ray angle-resolved photoemission. We find an anomaly in orbital ordering of the mobile electrons in {\gamma}-Al2O3/SrTiO3 which depopulates electron states in the top STO layer. This rearrangement of the mobile electron system pushes the electron density away from the interface that reduces its overlap with the interfacial defects and weakens the electron-phonon interaction, both effects contributing to the mobility boost. A crystal-field analysis shows that the band order alters owing to the symmetry breaking between the spinel {\gamma}-Al2O3 and perovskite SrTiO3. The band-order engineering exploiting the fundamental symmetry properties emerges as another route to boost the performance of oxide devices.
In magic angle twisted bilayer graphene, transport, thermodynamic and spectroscopic experiments pinpoint at a competition between distinct low-energy states with and without electronic order, as well as a competition between localized and delocalized charge carriers. In this study, we utilize Dynamical Mean Field Theory (DMFT) on the topological heavy Fermion (THF) model of twisted bilayer graphene to investigate the emergence of electronic correlations and long-range order in the absence of strain. We explain the nature of emergent insulating and correlated metallic states, as well as transitions between them driven by three central phenomena: (i) the formation of local spin and valley isospin moments around 100K, (ii) the ordering of the local isospin moments around 10K, and (iii) a cascadic redistribution of charge between localized and delocalized electronic states upon doping. At integer fillings, we find that low energy spectral weight is depleted in the symmetric phase, while we find insulating states with gaps enhanced by exchange coupling in the zero-strain ordered phases. Doping away from integer filling results in distinct metallic states: a "bad metal" above the ordering temperature, where coherence of the low-energy electronic excitations is suppressed by scattering off the disordered local moments, and a "good metal" in the ordered states with coherence of quasiparticles facilitated by isospin order. Upon doping, there is charge transfer between the localized and delocalized orbitals of the THF model such that they get periodically filled and emptied in between integer fillings. This charge reshuffling manifests itself in cascades of doping-induced Lifshitz transitions, local spectral weight redistributions and periodic variations of the electronic compressibility ranging from nearly incompressible to negative.
Strontium ruthenate Sr2RuO4 is an unconventional superconductor whose pairing symmetry has not been fully clarified, despite more than two decades of intensive research. Recent NMR Knight shift experiments have rekindled the Sr2RuO4 pairing debate by giving strong evidence against all odd-parity pairing states, including chiral p-wave pairing that was for a long time the leading pairing candidate. Here, we exclude additional pairing states by analyzing recent elastocaloric measurements [YS. Li et al., Nature 607, 276--280 (2022)]. To be able to explain the elastocaloric experiment, we find that unconventional even-parity pairings must include either large dx2−y2-wave or large {dxz∣dyz}-wave admixtures, where the latter possibility arises because of the body-centered point group symmetry. These {dxz∣dyz}-wave admixtures take the form of distinctively body-centered-periodic harmonics that have horizontal line nodes. Hence gxy(x2−y2)-wave and dxy-wave pairings are excluded as possible dominant even pairing states.