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Multi-node optical clock networks will enable future studies of fundamental physics and enable applications in quantum and classical communications as well as navigation and geodesy. We implement the first ever multi-node optical clock network with real-time, relative synchronization over free-space communication channels and precision on the order of 10 fs, realized as a three-node system in a hub-and-spoke topology. In this paper we describe the system and its performance, including a new, independent, out-of-loop verification of two-way optical time synchronization.

Recently evidence has emerged in the topological superconductor Fe-chalcogenide FeTe1-xSex for time-reversal symmetry breaking (TRSB), the nature of which has strong implications on the Majorana zero modes (MZM) discovered in this system. It remains unclear however whether the TRSB resides in the topological surface state (TSS) or in the bulk, and whether it is due to an unconventional TRSB superconducting order parameter or an intertwined order. Here by performing in superconducting FeTe1-xSex crystals both surface-magneto-optic-Kerr effect (SMOKE) measurements using a Sagnac interferometer and bulk magnetic susceptibility measurements, we pinpoint the TRSB to the TSS, where we also detect a Dirac gap. Further, we observe surface TRSB in non-superconducting FeTe1-xSex of nominally identical composition, indicating that TRSB arises from an intertwined surface ferromagnetic (FM) order. The observed surface FM bears striking similarities to the two-dimensional (2D) FM found in 2D van der Waals crystals, and is highly sensitive to the exact chemical composition, thereby providing a means for optimizing the conditions for Majorana particles that are useful for robust quantum computing., Comment: accepted version at Physical Review Letters

Elemental substitution is a proven method of Fermi level tuning in topological insulators, which is needed for device applications. Through static and time resolved photoemission, we show that in MnBi$_2$Te$_4$, elemental substitution of Bi with Sb indeed tunes the Fermi level towards the bulk band gap, making the material charge neutral at 35\% Sb concentration. For the first time, we are able to directly probe the excited state band structure at this doping level, and their dynamics, which show that the decay channels at the Fermi level are severely restricted. However, elemental substitution widens the surface state gap, which we attribute to the increase in antisite defects resulting from Sb substitution. This hypothesis is supported by DFT calculations that include defects, which show a sensitivity of the topological surface state to their inclusion. Our results emphasize the need for defect control if MnBi$_{2-x}$Sb$_x$Te$_4$ is to be used for device applications.

Intense debate has recently arisen regarding the photoinduced changes to the iron-chalcogenide superconductors, including the enhancement of superconductivity and a metastable state. Here, by employing high energy resolution, we directly observe the melting of superconductivity on ultrafast timescales. We demonstrate a distinctly nonequilibrium response on short timescales, where the gap fills in prior to the destruction of the superconducting peak, followed by a metastable response. We propose that the former is due to pair phase decoherence and speculate that the latter is due to the increase in double stripe correlations that are known to compete with superconductivity. Our results add to exciting new developments on the iron-based superconductors, indicating that the photoinduced metastable state possibly competes with superconductivity.

The idea of employing non-Abelian statistics for error-free quantum computing ignited interest in recent reports of topological surface superconductivity and Majorana zero modes (MZMs) in FeTe$_{0.55}$Se$_{0.45}$. An associated puzzle is that the topological features and superconducting properties are not observed uniformly across the sample surface. Understanding and practical control of these electronic inhomogeneities present a prominent challenge for potential applications. Here, we combine neutron scattering, scanning angle-resolved photoemission spectroscopy (ARPES), and microprobe composition and resistivity measurements to characterize the electronic state of Fe$_{1+y}$Te$_{1-x}$Se$_{x}$. We establish a phase diagram in which the superconductivity is observed only at sufficiently low Fe concentration, in association with distinct antiferromagnetic correlations, while the coexisting topological surface state occurs only at sufficiently high Te concentration. We find that FeTe$_{0.55}$Se$_{0.45}$ is located very close to both phase boundaries, which explains the inhomogeneity of superconducting and topological states. Our results demonstrate the compositional control required for use of topological MZMs in practical applications., Comment: Main text (18 pages, 5 figures, 50 references) combined with Supplementary (18 pages, 12 figures). Nat. Mater. (2021)

The topology of Weyl semimetals requires the existence of unique surface states. Surface states have been visualized in spectroscopy measurements, but their connection to the topological character of the material remains largely unexplored. 1T'-MoTe2, presents a unique opportunity to study this connection. This material undergoes a phase transition at 240K that changes the structure from orthorhombic (putative Weyl semimetal) to monoclinic (trivial metal), while largely maintaining its bulk electronic structure. Here we show from temperature-dependent quasiparticle interference measurements that this structural transition also acts as a topological switch for surface states in 1T'-MoTe2. At low temperature, we observe strong quasiparticle scattering, consistent with theoretical predictions and photoemission measurements for the surface states in this material. In contrast, measurements performed at room temperature show the complete absence of the scattering wavevectors associated with the trivial surface states. These distinct quasiparticle scattering behaviors show that 1T'-MoTe2 is ideal for separating topological and trivial electronic phenomena via temperature dependent measurements.

The phase diagram associated with the high Tc superconductors is complicated by an array of different ground states. The parent material represents an antiferromagnetic insulator but with doping superconductivity becomes possible with transition temperatures previously thought unattainable. The underdoped region of the phase diagram is dominated by the so-called pseudogap phenomena whereby in the normal state the system mimics superconductivity in its spectra response but does not show the complete loss of resistivity associated with the superconducting state. An understanding of this regime presents one of the great challenges for the field. In the present study we revisit the structure of the phase diagram as determined in photoemission studies. By careful analysis of the role of nanoscale inhomogeneities in the overdoped region we are able to more carefully separate out the gaps due to the pseudogap phenomena from the gaps due to the superconducting transition. Within a mean field description we are thus able to link the magnitude of the gap directly to the Heisenberg exchange interaction term, $J\sum{s_i \cdot s_j}$, contained in the $t-J$ model. This approach provides a clear indication that the pseudogap is that associated with spin singlet formation., Comment: revised to include supplementary section and correct references in Fig. 5

We directly measure the electronic structure of twisted graphene/MoS2 van der Waals heterostructures, in which both graphene and MoS2 are monolayers. We use cathode lens microscopy and microprobe angle-resolved photoemission spectroscopy measurements to image the surface, determine twist angle, and map the electronic structure of these artificial heterostructures. For monolayer graphene on monolayer MoS2, the resulting band structure reveals the absence of hybridization between the graphene and MoS2 electronic states. Further, the graphene-derived electronic structure in the heterostructures remains intact, irrespective of the twist angle between the two materials. In contrast, however, the electronic structure associated with the MoS2 layer is found to be twist-angle dependent; in particular, the relative difference in the energy of the valence band maximum at {\Gamma} and K of the MoS2 layer varies from approximately 0 to 0.2 eV. Our results suggest that monolayer MoS2 within the heterostructure becomes predominantly an indirect bandgap system for all twist angles except in the proximity of 30 degrees. This result enables potential bandgap engineering in van der Waals heterostructures comprised of monolayer structures., Comment: 20 pages including supplementary materials

We report ARPES and a set of in situ STM measurements on a narrow-terrace-width vicinal Cu(111) crystal surface, Cu(775), whose vicinal cut lies close to the transition between terrace and step modulation. These measurements show sharp zone-folding (or Umklapp) features with a periodicity in k||, indicating that the predominant reference plane is that of Cu(775), i.e. that the surface is predominately step-modulated. Our measurements also show variation in Umklapp intensity with photon energy, which is consistent with prior ARPES experiments on other vicinal Cu(111) surfaces and in agreement with our designation of the state as being step modulated. The measurements also show a weak terrace-modulated state, which, based on several characteristics, we attribute to the presence of terrace widths larger than the ideal terrace width. By measuring the intensity ratio of the two distinct surface-state modulations from PE and the terrace-width distribution from STM, we derive a value for the terrace width, at which the surface-state switches between the two modulations., Comment: 13 pages, 5 figures

We report on a new surface phase of the Co-vicinal-Cu(111) system which exhibits self-assembled uniform Co quantum wires that are stable at 300K. STM-imaging measurements show that wires will self-assemble within a narrow range of Co coverage and, within this range, the wires increase in length as coverage is increased. The STM images show that the wires form along the leading edge of the step rise, differentiating it from previously theoretically predicted atomic-wire phases. The formation of relatively long laterally un-encapsulated one- and two-atom wires also differentiates it from past experimentally observed step-island formation. Furthermore, our experiments also show directly that the Co wires coexist with another Co phase that had been previously predicted for growth on Cu(111). Our observations allow us to comment on the formation kinetics of the atomic-wire phase and on the fit of our data to a recently developed lattice-gas model., Comment: 14 pages, 5 figures

Density functional theory (DFT) has been immensely successful in its ability to predict physical properties, and, in particular, structures of condensed matter systems. Here, however, we show that DFT qualitatively fails to predict the dimerized structural phase for a monatomic Co wire that is self-assembled on a vicinal, i.e. stepped, Cu(111) substrate. To elucidate the nature of this failure, we compute the energetics of a Co chain on a Cu surface, step, notch, and embedded in bulk. The results demonstrate that increasing Co coordination extinguishes the dimerization, indicating that the failure of DFT for Co on the Cu step arises from excessive hybridization, which both weakens the ferromagnetic correlations that drive the dimerization and increases the bonding that opposes dimerization. Additionally, we show that including local interactions via DFT+U or DFT+DMFT does not restore the dimerization for the step-substrate supported wire, though the Co wire does dimerize in DFT+DMFT for the isolated vacuum case. This system can serve as a benchmark for future electronic structure methods., Comment: 18 pages, 7 figures

Using low-temperature scanning tunneling microscopy, we demonstrate an unambiguous 1-D system that surprisingly undergoes a CDW instability on a metallic substrate. Our ability to directly and quantitatively measure the structural distortion of this system provides an accurate reference for comparison with first principles theory. In comparison to previously proposed physical mechanisms, we attribute this particular 1-D CDW instability to a ferromagnetic state. We show that though the linear arrayed dimers are not electronically isolated, they are magnetically independent, and hence can potentially serve as a binary spin-memory system., Comment: Includes Supplementary Information