In low-dimensional superconductors, the interplay between quantum confinement and interfacial hybridization effects can reshape Cooper-pair wavefunctions and give rise to unconventional superconducting states. Here we use plasma-free confinement epitaxy assisted by a carbon buffer layer to synthesize a gallium trilayer sandwiched between graphene and a 6H-SiC(0001) substrate. Within this confined gallium layer, we demonstrate interfacial Ising-type superconductivity driven by atomic orbital hybridization. Electrical transport measurements reveal that the in-plane upper critical magnetic field reaches ~21.98 T at T = 400 mK, approximately 3.38 times the Pauli paramagnetic limit. Angle-resolved photoemission spectroscopy measurements, combined with theoretical calculations, confirm the presence of split Fermi surfaces with Ising-type spin textures at the K and K' valleys of the confined gallium layer, originating from strong hybridization with the SiC substrate. This work establishes a strategy for realizing unconventional pairing wavefunctions through the synergistic combination of quantum confinement and interfacial hybridization effects.
The interplay among orbital-selective Mott physics, Hund's coupling, tunable structural motifs, and Kondo-like scattering establishes a compelling paradigm for understanding and engineering correlated multi-orbital systems, as vividly exemplified by nickelate superconductors. Here, using high-resolution angle-resolved photoemission spectroscopy combined with theoretical calculations, we systematically investigate the electronic properties of trilayer nickelates. In La4Ni3O10, we observe pronounced interorbital hybridization, whereas in Pr4Ni3O10, the flat d_(z^2 ) band becomes markedly incoherent and diminishes in spectral weight. By contrast, the dispersive d_(x^2-y^2 ) bands retain coherence in both compounds. This striking incoherence/coherence dichotomy identifies an orbital-selective Mott phase modulated by the interlayer Ni-O-Ni bonding angle. The depletion of the d_(z^2 ) orbitals further frustrates the interorbital hybridization and influences the density-wave transition in Pr4Ni3O10. Moreover, the density-wave gap is substantially reduced in Pr4Ni3O10, likely due to extra scattering channels provided by the local moments of Pr3+ cations. Our findings elucidate the intricate interplay among lattice, orbital, spin, and electronic degrees of freedom and reveal a feasible structural control parameter for the multi-orbital correlated state in trilayer nickelates, which provide a concrete framework for understanding the emergence of superconductivity under high pressure.
The physical properties of magnetic topological materials are strongly influenced by their nontrivial band topology coupled with the magnetic structure. Co3Sn2S2 is a ferromagnetic kagome Weyl semimetal displaying giant intrinsic anomalous Hall effect which can be further tuned via elemental doping, such as Ni substitution for Co. Despite significant interest, the exact valency of Co and the magnetic order of the Ni dopants remained unclear. Here, we report a study of Ni-doped Co3Sn2S2 single crystals using synchrotron-based X-ray magnetic circular dichroism (XMCD), X-ray photoelectron emission microscopy (XPEEM), and hard/soft X-ray photoemission spectroscopy (XPS) techniques. We confirm the presence of spin-dominated magnetism from Co in the host material, and also the establishment of ferromagnetic order from the Ni dopant. The oxygen-free photoemission spectrum of the Co 2p core levels in the crystal well resembles that of a metallic Co film, indicating a Co0+ valency. Surprisingly, we find the electron filling in the Co 3d state can reach 8.7-9.0 electrons in these single crystals. Our results highlight the importance of element-specific X-ray spectroscopy in understanding the electronic and magnetic properties that are fundamental to a heavily studied Weyl semimetal, which could aid in developing future spintronic applications based on magnetic topological materials.
The resurgence of interest in Kondo insulators has been driven by two major mysteries: the presence of metallic surface states and the observation of quantum oscillations. To further explore these mysteries, it is crucial to investigate another similar system beyond the two existing ones, SmB 6 and YbB 12 . Here, we address this by reporting on a Kondo insulator, U 3 Bi 4 Ni 3 . Our transport measurements reveal that a surface state emerges below 250 kelvin and dominates transport properties below 150 kelvin, which is well above the temperature scale of SmB 6 and YbB 12 . At low temperatures, the surface conductivity is about one order of magnitude higher than the bulk. The robustness of the surface state indicates that it is inherently protected. The similarities and differences between U 3 Bi 4 Ni 3 and the other two Kondo insulators will provide valuable insights into the nature of metallic surface states in Kondo insulators and their interplay with strong electron correlations.
Berry curvature and spin texture are representative tuning parameters that govern spin-orbit coupling-related physics and are also the foundation for future device applications. Here, we investigate the impact of the Sb-to-Bi ratio on shaping the electronic band structure and its correlated first- and second-harmonic magneto-transport signals in the intrinsic magnetic topological insulator Mn(Bi1-xSbx)(2)Te-4. First-principles calculations reveal that the introduction of Sb not only triggers a topological phase transition but also changes the integral of the Berry curvature at the shifted Fermi level, which leads to the reversal of the anomalous Hall resistance polarity for Sb fractions x > 0.67. Moreover, it also induces the opposite spin splitting of the valence bands compared to the Sb-free host, and the resulting clockwise/counterclockwise spin chirality gives rise to a tunable unidirectional second-harmonic anomalous Hall response. Our findings pave the way for constructing chiral spin-orbitronic devices through band structure engineering.
Berry curvature and spin texture are representative tuning parameters that govern spin-orbit coupling–related physics and are also the foundation for future device applications. Here, we investigate the impact of the Sb-to-Bi ratio on shaping the electronic band structure and its correlated first- and second-harmonic magneto-transport signals in the intrinsic magnetic topological insulator Mn(Bi 1− x Sb x ) 2 Te 4 . First-principles calculations reveal that the introduction of Sb not only triggers a topological phase transition but also changes the integral of the Berry curvature at the shifted Fermi level, which leads to the reversal of the anomalous Hall resistance polarity for Sb fractions x > 0.67. Moreover, it also induces the opposite spin splitting of the valence bands compared to the Sb-free host, and the resulting clockwise/counterclockwise spin chirality gives rise to a tunable unidirectional second-harmonic anomalous Hall response. Our findings pave the way for constructing chiral spin-orbitronic devices through band structure engineering.
Correlated kagome materials exhibit a compelling interplay between lattice geometry, electron correlation, and topology. In particular, the flat bands near the Fermi level provide a fertile playground for novel many-body states. Here we investigate the electronic structure of CsCr3Sb5 using high-resolution angle-resolved photoemission spectroscopy and ab-initio calculations. Our results suggest that Cr 3d electrons are intrinsically incoherent, showing strong electron correlation amplified by Hund's coupling. Notably, we identify incipient flat bands close to the Fermi level, which are expected to significantly influence the electronic properties of the system. Across the density-wave-like transition at 55 K, we observe a drastic enhancement of the electron scattering rate, which aligns with the semiconducting-like property at high temperatures. These findings establish CsCr3Sb5 as a strongly correlated Hund's metal with incipient flat bands near the Fermi level, which provides an electronic basis for understanding its novel properties compared to the weakly correlated AV3Sb5.
MnBi2Te4-based superlattices not only enrich the materials family of magnetic topological insulators, but also offer a platform for tailoring magnetic properties and interlayer magnetic coupling through the strategic insertion layer design. Here, we present the electrical and magnetic characterization of (Bi1-xSbx)2Te3-intercalated MnBi2Te4 multilayers grown by molecular beam epitaxy. By precisely adjusting the Sb-to-Bi ratio in the spacer layer, the magneto-transport response is modulated, unveiling the critical role of Fermi level tuning in optimizing the anomalous Hall signal and reconfiguring the magnetic ground state. Moreover, by varying the interlayer thickness, tunable magnetic coupling is achieved, enabling precise control over ferromagnetic and antiferromagnetic components. These findings pave the way for the exploration of versatile magnetic topological phases in quantum materials systems.
This study investigates the intrinsic magnetism and field‐driven spin alignment in NiI 2 using X‐ray absorption spectroscopy and X‐ray magnetic circular dichroism (XMCD). NiI 2 , a van der Waals material, exhibits helimagnetic and type‐II multiferroic behavior. This study reveals robust XMCD signals across paramagnetic, antiferromagnetic, and helimagnetic phases under applied out‐of‐plane fields up to 6 T, while no net moment emerges at zero field. Atomic multiplet calculations confirm a covalent Ni 3 d ground state with a significantly reduced spin moment. The results establish the intrinsic nature of NiI 2 's magnetism and clarify its field‐driven spin alignment mechanism. This comprehensive spectroscopic characterization lays the foundation for future applications of NiI 2 in advanced spintronic and multiferroic devices, despite challenges posed by its low transition temperature in the monolayer limit. Future research should focus on enhancing its critical temperature through doping, strain engineering, or heterostructure fabrication.
The origin of the high temperature superconductivity in the iron-based superconductors remains elusive after being extensively studied for more than a decade. Determination of the pairing symmetry is essential in understanding the superconductivity mechanism. In the iron-based superconductors that have hole pockets around the Brillouin zone center and electron pockets around the zone corners, the pairing symmetry is generally considered to be s$_\pm$, endowing a sign change in the superconducting gap between the hole and electron pockets. For the iron-based superconductors with only hole pockets, however, a couple of pairing scenarios have been proposed but the exact symmetry is still highly controversial. Here we report our determination of the pairing symmetry in KFe$_2$As$_2$ which is a prototypical iron-based superconductor with hole pockets both around the zone center and around the zone corners. By taking laser-based angle resolved photoemission measurements with super-high resolution and at ultra-low temperature, we have precisely determined the superconducting gap distribution and identified the locations of the gap nodes on all the Fermi surface around the zone center and the zone corners. The complete superconducting gap structure, in combination with the observation of the spin resonance in neutron scattering, provides strong evidence on the s$_\pm$ pairing symmetry in KFe$_2$As$_2$ with a gap sign reversal between the hole pockets around the zone center and the hole pockets around the zone corners. These results unify the pairing symmetry in the hole-doped iron-based superconductors and point to the spin fluctuation as the pairing glue in generating superconductivity.
The surface of three-dimensional materials provides an ideal and versatile platform to explore quantum-confined physics. Here, we systematically investigate the electronic structure of Na-intercalated CrTe2, a van der Waals antiferromagnet, using angle-resolved photoemission spectroscopy and ab initio calculations. The measured band structure deviates from the calculation of bulk NaCrTe2 but agrees with that of ferromagnetic monolayer CrTe2. Consistently, we observe unexpected exchange splitting of the band dispersions, persisting well above the Néel temperature of bulk NaCrTe2. We argue that NaCrTe2 features a quantum-confined 2D ferromagnetic state in the topmost surface layer due to strong ferromagnetic correlation in the CrTe2 layer. Moreover, the exchange splitting and the critical temperature can be controlled by surface doping of alkali-metal atoms, suggesting the feasibility of tuning the surface ferromagnetism. Our work not only presents a simple platform for exploring tunable 2D ferromagnetism but also provides important insights into the quantum-confined low-dimensional magnetic states.
Kagome materials exhibit many novel phenomena emerging from the interplay between lattice geometry, electronic structure, and topology. A prime example is the vanadium-based kagome materials AV3Sb5 (A = K, Rb, and Cs) with superconductivity and unconventional charge-density wave (CDW). More interestingly, the substitution of vanadium by chromium further introduces magnetism and enhances the correlation effect in CsCr3Sb5 which likewise exhibits superconductivity under pressure and competing density-wave state. Here we systematically investigate the electronic structure of CsCr3Sb5 using high-resolution angle-resolved photoemission spectroscopy (APRES) and ab-initio calculations. Overall, the measured electronic structure agrees with the theoretical calculation. Remarkably, Cr 3d orbitals exhibit incoherent electronic states and contribute to incipient flat bands close to the Fermi level. The electronic structure shows a minor change across the magnetic transition at 55 K, suggesting a weak interplay between the local magnetic moment and itinerant electrons. Furthermore, we reveal a drastic enhancement of the electron scattering rate across the magnetic transition, which is relevant to the semiconducting-like transport property of the system at high temperatures. Our results suggest that CsCr3Sb5 is a strongly correlated Hund's metal with incipient flat bands near the Fermi level, which provides an electronic basis for understanding its novel properties in comparison to the non-magnetic and weakly correlated AV3Sb5.
Bead-based immunoassays are multiparametric analysis allowing for the simultaneous quantification of a large number of biomarkers within a single sample. Mass cytometry is an emerging cytometric technique that offers a high multiplexing capacity in a high-throughput setting but has not yet been applied to bead-based assays. In this study, we developed a multiplex bead-based immunoassay of cytokines and CD163 designed for mass cytometry (MC). A set of 11 types of lanthanide-encoded microbeads were synthesized by two-stage dispersion polymerization as classifier candidates for the assay. These beads were then decorated with different Abs on the surface to capture the target cytokines in solution. Gold nanoparticles were employed as reporters to identify the binding of target cytokines on the classifier surface. As a proof-of-concept study, we first developed four-plex and nine-plex assays of mixtures of cytokines in standard solutions. The MC signal intensities of these immunoassays were responsive to the concentration differences in the standard solutions with high detection sensitivities at low analyte concentrations. Finally, we examined a sample of peripheral blood mononuclear cells (PBMCs) with the nine-plex assay, comparing an unstimulated sample with a sample stimulated to promote cytokine secretion.
Crystal geometry can greatly influence the emergent properties of quantum materials. As an example, the kagome lattice is an ideal platform to study the rich interplay between topology, magnetism, and electronic correlation. In this work, combining high-resolution angle-resolved photoemission spectroscopy and ab-initio calculation, we systematically investigate the electronic structure of XMn6Sn6 (X = Dy, Tb, Gd, Y) family compounds. We observe the Dirac fermion and the flat band arising from the magnetic kagome lattice of Mn atoms. Interestingly, the flat band locates in the same energy region in all compounds studied, regardless of their different magnetic ground states and 4f electronic configurations. These observations suggest a robust Mn magnetic kagome lattice across the XMn6Sn6 family, thus providing an ideal platform for the search and investigation on new emergent phenomena in magnetic topological materials.
Lanthanide nanoparticles (LnNPs) have the potential to be used as high-sensitivity mass tag reporters in mass cytometry immunoassays. For this application, however, the LnNPs must be made colloidally stable in aqueous buffers, demonstrate minimal non-specific binding to cells, and have functional groups to attach antibodies or other targeting agents. One possible approach to address these requirements is by using lipid coating to modify the surface of the LnNPs. In this work, 39 nm diameter NaYF4:Yb, Er NPs (LnNPs) were coated with a lipid formulation consisting of egg sphingomyelin, 1,2-dioleoyl-sn-glycero-3-phosphocholine, 1,2-dioleoyl-3-trimethylammonium propane, cholesterol-(polyethylene glycol-600), and 1,2-distearoyl-sn-glycero-3-phosphoethanolamine-N-[biotinyl(polyethylene glycol)-2000]. The resulting biotinylated lipid-coated LnNPs were characterized by dynamic light scattering to determine the hydrodynamic size and stability in phosphate buffered saline, and the composition of the lipid coatings was quantified by liquid chromatography-tandem mass spectrometry. The specific and non-specific binding of the biotinylated lipid-coated LnNPs to a model system of functionalized polystyrene microbeads were then tested by both suspension and imaging mass cytometry. We found that targeted binding with minimal non-specific binding can be achieved with the lipid-coated LnNPs and that the lipid composition of the coating has an impact on the performance of the LnNPs as mass cytometry reporters. These results additionally establish the importance of quantifying the composition of lipid-coated nanomaterials to optimize them more effectively for their desired application.
The study of magnetic order in few- and monolayer van der Waals materials poses a challenge to the most commonly employed magnetic characterization techniques as they normally lack magnetic sensitivity and/or lateral resolution enabling their thickness-dependent probing. Here we demonstrate the usefulness of x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr L2,3 and Te M 5 edges, for the study of the ferromagnetic semiconductor CrSiTe3 (CST) in the form of single- and few-layer flakes. By scanning the sample under the incident x-ray beam, a map of the exfoliated system was obtained, which reproduced the optical micrographs showing the detailed distribution and thicknesses of the flakes. In this way, XAS/XMCD was performed at selected sample areas, revealing the thickness-resolved spectroscopic and magnetic properties of the flakes, such as the spin and orbital magnetic moments. The spin moment, in line with the saturation field, is decreasing with film thickness, revealing a single-domain and out-of-plane magnetization for the thinnest films. For CST, the electronic properties are governed by the strong covalent bond between the Cr 3d(e g ) and Te 5p states, giving rise to a superexchange scenario. We observed a gradually increasing ratio of orbital to spin moment for thinner flakes, which could be due to a further increase of the covalent mixing. Hysteresis loops were recorded at the Cr L 3 edge, showing an open loop for 10 down to ∼3 layers, while the bulk shows a wasp-waist shaped loop. With the transition temperature from the soft to the hard ferromagnetic state decreasing with thickness, the monolayer shows a narrowed, closed loop at 10 K, suggesting its transition temperature > 10 K. Our study demonstrates the unique capabilities of XAS/XMCD for the study of few-layer van der Waals magnets, highlighting the interplay between electron correlation and ferromagnetism in CST.
Bead-based assays in flow cytometry are multiplexed analytical techniques that allow rapid and simultaneous detection and quantification of a large number of analytes from small volumes of samples. The development of corresponding bead-based assays in mass cytometry (MC) is highly desirable since it could increase the number of analytes detected in a single assay. The microbeads for these assays have to be labeled with metal isotopes for MC detection. One must also be able to functionalize the bead surface with affinity reagents to capture the analytes. Metal-encoded polystyrene microbeads prepared by multi-stage dispersion polymerization can produce effective isotopic signals in MC with relatively small bead-to-bead variations. However, functionalizing this microbead surface with bioaffinity agents remains challenging, possibly due to the interference of the steric-stabilizing PVP corona on the microbead surface. Here, we report a systematic investigation of a silica coating approach to coat Eu-encoded microbeads with thin silica shells, to functionalize the surface with amino groups, and to introduce bioaffinity agents. We examine the effect of silica shell roughness on the bioconjugation capacity and the effect of silica shell thickness on signal quality in MC measurements. To limit non-specific binding, we converted the amino groups on the microbead surface to carboxylic acid groups. Antibodies were effectively attached to microbead by first conjugating NeutrAvidin to the carboxyl-modified bead surface and then attaching biotinylated antibodies to the NeutrAvidin-modified bead surface. The antibody-modified microbeads can specifically capture antigens, which were marked with isotopic labels, and generate strong signals in MC. These are promising results for the development of bead-based assays in MC.
We investigate transport properties and the electronic structure of BiCuSO, a thermoelectric material which was predicted as a possible parent compound for unconventional superconductivity. For the p-type BiCuSO samples studied in this paper, our transport measurements show metallic behavior down to 2 K, and we observe an increase of saturated magnetic moment around 4 K, which could be due to the reorientation of the magnetic easy axis. Using angle-resolved photoemission spectroscopy measurements, we acquired the comprehensive electronic structure of BiCuSO including the predicted flat band, and by carrying out photon polarization dependent measurements we further investigated the orbital characters of bands near the Fermi level. Compared with its sister compound, BiCuSeO, we find the flat band could be the origin of high figure of merit (ZT) value in the BiCuChO (Ch = S, Se) family.
Topological insulators (TIs) provide intriguing prospects for the future of spintronics due to their large spin-orbit coupling and dissipationless, counter-propagating conduction channels in the surface state. The combination of topological properties and magnetic order can lead to new quantum states including the quantum anomalous Hall effect that was first experimentally realized in Cr-doped (Bi,Sb)2 Te3 films. Since magnetic doping can introduce detrimental effects, requiring very low operational temperatures, alternative approaches are explored. Proximity coupling to magnetically ordered systems is an obvious option, with the prospect to raise the temperature for observing the various quantum effects. Here, an overview of proximity coupling and interfacial effects in TI heterostructures is presented, which provides a versatile materials platform for tuning the magnetic and topological properties of these exciting materials. An introduction is first given to the heterostructure growth by molecular beam epitaxy and suitable structural, electronic, and magnetic characterization techniques. Going beyond transition-metal-doped and undoped TI heterostructures, examples of heterostructures are discussed, including rare-earth-doped TIs, magnetic insulators, and antiferromagnets, which lead to exotic phenomena such as skyrmions and exchange bias. Finally, an outlook on novel heterostructures such as intrinsic magnetic TIs and systems including 2D materials is given.