Orbital-selective correlations have been observed to play an important role in Fe-based superconductors. Here, in contrast to previous site-local Mott transition-based origins, we present a band-theory-based mechanism for orbital-selective physics in monolayer FeSe, for which only electron pockets appear. Underlying our mechanism is the observation in density functional theory (DFT) calculations that around the M point in the Brillouin zone, antiferromagnetic fluctuations are strongly coupled to electrons in x2 − y2 orbitals but weakly coupled to those in {xz, yz} orbitals. Symmetry-arguments reveal that this orbital selective coupling originates from the different intertwined orbital and Fe-site sublattice Bloch wavefunctions for these two sets of orbitals at the M point, specifically, the x2 − y2 orbitals can be Fe-site localized. The strong coupling of electrons in x2 − y2 orbitals to the magnetic fluctuations enables orbital-selective electronic renormalizations that can account for important features of our angle-resolved photoemission spectroscopy measurements. Our symmetry-required mechanism for orbital selective physics can be generalized to a range of crystal space groups with four-fold and six-fold screw axes. Orbital-selective correlations are crucial in understanding Fe-based superconductors, yet their origins remain debated. Here, the authors propose a band-theory-based mechanism for orbital-selective physics in monolayer FeSe, revealing that antiferromagnetic fluctuations selectively couple to x2 − y2 orbitals, offering broader insights for orbital-selective systems with four-fold and six-fold symmetry axes.

Single-layer FeSe on SrTiO3(001) substrates shows a superconducting transition temperature much higher than that of bulk FeSe, which has been attributed to factors such as electron doping, interfacial electron-phonon coupling, and electron correlations. To pinpoint the primary driver, we grew single-layer FeSe films on SrTiO3(001) substrates with coexisting TiO2 and SrO surface terminations. Scanning tunneling spectroscopy revealed a larger superconducting gap (17.0 meV) on the TiO2-termination than on the SrO-termination (10.5 meV). Tunneling spectroscopy also showed a larger work function on the SrO surface, resulting in reduced charge transfer to FeSe, as confirmed by angle-resolved photoemission spectroscopy. Scanning transmission electron microscopy further revealed distinctive interfacial atomic-scale structures, with the Se-Fe-Se tetrahedral angle changing from 109.5° on the SrO-termination to 104.9° on the TiO2-termination. Compared to dynamical mean field theory calculations, our results indicate that enhanced superconductivity in single-layer FeSe/TiO2 arises from optimal electron correlations, in addition to sufficient charge transfer from the substrate.

While a predictive theory for unconventional superconductivity in Fe-based superconductors remains elusive, an extensively debated aspect is the interaction between phonons and strongly correlated electrons, and its potential role in the pairing mechanism. Here, through the combination of first principles dynamical mean field theory calculations and epitaxial growth of the single-layer FeX (X=Se, S, Te) on SrTiO_3 (STO)(001) substrate, which facilitates the controlled distortion of the FeX_4 tetrahedron, we demonstrate an unique superconducting dome where the superconducting gap peaks at a `magic' angle of the FeX_4 tetrahedron and the electron-phonon coupling (EPC) for the A_1g mode is maximized for the FeSe film. Our findings uncover a significant role of electronic correlations in strengthening Cooper pairing in unconventional superconductors by enhancing EPC.

In iron-based superconductors, the two Fe atoms in the unit cell are typically related by crystal symmetries; therefore, we expect no intra-unit cell variations in the superconducting gap. However, recent experiments have challenged this expectation, reporting intra-unit cell variations in the gap with an unusual particle-hole asymmetry. Here, we examine the origin of this asymmetry between the two Fe sublattices in monolayer FeSe grown on SrTiO$_3$. We reveal that, in addition to the substrate-induced broken inversion symmetry, substrate nematic symmetry breaking is key to observing this asymmetry. We further identify two possible mechanisms through which this can occur. The first is through an odd-parity gap function that coexists with an extended $s$-wave function. The second is via a nodeless $d$-wave gap function that develops in the presence of a symmetry-breaking substrate. We argue that the latter mechanism is more physical. To test our theory, we performed scanning tunneling spectroscopy measurements across the nematic domain walls, which exhibit a clear enhancement of the asymmetry between the two Fe sublattices. In addition, we reveal that the observed sublattice particle-hole asymmetry is associated with odd-frequency pairing correlations, providing an experimental realization of this unusual pairing correlation.

We report radio-frequency measurements of quality factors and temperature mapping of a nitrogen doped Nb superconducting RF cavity. Cavity cutouts of hot and cold spots were studied with low temperature scanning tunneling microscopy and spectroscopy, X-ray photoelectron spectroscopy and secondary electron microscopy. Temperature mapping revealed a substantial reduction of the residual resistance upon cooling the cavity with a greater temperature gradient and hysteretic losses at the quench location, pointing to trapped vortices as the dominant source of residual surface resistance. Analysis of the tunneling spectra in the framework of a proximity effect theory shows that hot spots have a reduced pair potential and a wider distribution of the contact resistance between the Nb and the top Nb oxide. Alone, these degraded superconducting properties account for a much weaker excess dissipation as compared with the vortex contribution. Based on the correlation between the quasiparticle density of states and temperature mapping, we suggest that degraded superconducting properties may facilitate vortex nucleation or settling of trapped flux during cooling the cavity through the critical temperature.

Chemical pressure from the isovalent substitution of Se by a larger Te atom in the epitaxial film of iron chalcogenide FeSe can effectively tune its superconducting, topological, and magnetic properties. However, such substitution during epitaxial growth inherently leads to defects and structural inhomogeneity, making the determination of alloy composition and atomic sites for the substitutional Te atoms challenging. Here, we utilize machine learning to distinguish between Se and Te atoms in scanning tunneling microscopy images of single-layer FeSe1−xTex on SrTiO3(001) substrates. Defect locations are first identified by analyzing spatial-dependent dI/dV tunneling spectra using the K-means clustering method. After excluding the defect regions, the remaining dI/dV spectra are further analyzed using the singular value decomposition method to determine the Se/Te ratio. Our findings demonstrate an effective and reliable approach for determining alloy composition and atomic-scale electronic inhomogeneity in superconducting single-layer iron chalcogenide films.

Scanning tunneling microscopy (STM) is a powerful technique for imaging atomic structure and inferring information on local elemental composition, chemical bonding, and electronic excitations. However, a plain visual analysis of STM images can be challenging for such determination in multicomponent alloys, particularly beyond the diluted limit due to chemical disorder and electronic inhomogeneity. One viable solution is to use machine learning to analyze STM data and identify hidden patterns and correlations. Here, we apply this approach to determine the Se/S concentration in superconducting single-layer FeSe1-xSx alloys epitaxially grown on SrTiO3(001) substrates via molecular beam epitaxy. First, the K-means clustering method is applied to identify defect-related dI/dV tunneling spectra taken by current imaging tunneling spectroscopy. Then, the Se/S ratio is calculated by analyzing the remaining spectra based on the singular value decomposition method. Such analysis provides an efficient and reliable determination of alloy composition and further reveals the correlations of nanoscale chemical inhomogeneity to superconductivity in single-layer iron chalcogenide films.

Kagome lattice hosts a plethora of quantum states arising from the interplay of topology, spin-orbit coupling, and electron correlations. Here, we report symmetry-breaking electronic orders tunable by an applied magnetic field in a model Kagome magnet FeSn consisting of alternating stacks of two-dimensional Fe 3 Sn Kagome and Sn 2 honeycomb layers. On the Fe 3 Sn layer terminated FeSn thin films epitaxially grown on SrTiO 3 (111) substrates, we observe trimerization of the Kagome lattice using scanning tunneling microscopy/spectroscopy, breaking its six-fold rotational symmetry while preserving the translational symmetry. Such a trimerized Kagome lattice shows an energy-dependent contrast reversal in dI/dV maps, which is significantly enhanced by bound states induced by Sn vacancy defects. This trimerized Kagome lattice also exhibits stripe modulations that are energy-dependent and tunable by an applied in-plane magnetic field, indicating symmetry-breaking nematicity from the entangled magnetic and charge degrees of freedom in antiferromagnet FeSn.

By substituting S into single-layer FeSe/SrTiO3, chemical pressure is applied to tune its paramagnetic state that is modeled as an incoherent superposition of spin-spiral states. The resulting electronic bands resemble an ordered checkerboard antiferromagnetic structure, consistent with angle-resolved photoemission spectroscopy measurements. Scanning tunneling spectroscopy reveals a gap evolving from U-shaped for FeSe to V-shaped for FeS with decreasing size, attributed to a d-wave superconducting state for which nodes emerge once the gap size is smaller than the effective spin-orbit coupling.

We use scanning tunneling microscopy (STM) and spectroscopy (STS), and x-ray photoelectron spectroscopy (XPS) to investigate the effect of nitrogen doping on the surface electronic and chemical structures of cutouts from superconducting $\mathrm{Nb}$ radio-frequency cavities. The goal of this work is to get insights into the fundamental physics and materials mechanisms behind the striking decrease of the surface resistance with the radio-frequency magnetic field, which has been observed on $N$-doped $\mathrm{Nb}$ cavities. Our XPS measurements reveal significantly more oxidized $\mathrm{Nb}$ $3d$ states and a thinner metallic suboxide layer on the $N$-doped $\mathrm{Nb}$ surfaces, which is also confirmed by tunneling spectroscopy measurements. In turn, tunneling measurements performed on native surfaces as well as on $\mathrm{Ar}$-ion sputtered surfaces allow us to separate the effect of $N$ doping on the surface-oxide layer from that on the density of states in the bulk. Analysis of our tunneling spectra in the framework of a model of a proximity-coupled normal layer at the surface [A. Gurevich and T. Kubo, Phys. Rev. B 96, 184515 (2017)] is consistent with the hypothesis that $N$-doping ameliorates lateral inhomogeneities of superconducting properties on the surface and shrinks the metallic suboxide layer. For the $\mathrm{Ar}$ sputtered surfaces, we also find evidence that $N$ doping changes the contact resistance between the metallic suboxide and the bulk niobium toward an optimum value corresponding to a minimum surface resistance. The totality of our experimental data suggests that the $N$ doping provides an effective tuning of the density of states in such a way that it can result in a decrease of the surface resistance with the radio-frequency field, as predicted by calculations of the nonlinear low-frequency electromagnetic response of dirty superconductors. Furthermore, STM imaging of vortex cores shows a slightly reduced average superconducting gap and a shorter coherence length in the $N$-doped $\mathrm{Nb}$ samples as compared to typically prepared $\mathrm{Nb}$ samples, indicating a stronger impurity scattering caused by nitrogen doping in a moderately disordered material.

We have performed the first-principles study of adsorption of alkali metals like lithium, sodium and potassium on graphene. As first-principles methods we have chosen Hartree-Fock method and density functional theory (DFT) method. We have studied the variation of energy of grapheme clusters on sizes of the graphene clusters. Our findings show that the energy of graphene clusters increases with the size of the clusters and for the cluster size more than 30 carbon atoms the energy per carbon atom remains almost constant. This shows that the graphene clusters are stable with respect to energy for the larger size of clusters. The adsorption of alkali metals on the H-grpahene clusters have been studied. The adsorption energy of alkali metal atoms (Li, Na and K) on H-graphene increases on increasing the size of H-graphene cluster. The dependence of the computed adsorption energies of Li, Na and K atoms on the size of H-graphene clusters and the presence of large dipole moments in the adatoms-H-graphene system exhibit the ionic character of the alkali metal adatom-H-graphene interaction. Our findings on the adsorption energy of the alkali metals on H-graphene clusters agree with the previously reported data.