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We present the development of a versatile apparatus for 6.2 eV laser-based time and angle-resolved photoemission spectroscopy with micrometer spatial resolution (time-resolved μ-ARPES). With a combination of tunable spatial resolution down to ∼11 μm, high energy resolution (∼11 meV), near-transform-limited temporal resolution (∼280 fs), and tunable 1.55 eV pump fluence up to 3 mJ/cm2, this time-resolved μ-ARPES system enables the measurement of ultrafast electron dynamics in exfoliated and inhomogeneous materials. We demonstrate the performance of our system by correlating the spectral broadening of the topological surface state of Bi2Se3 with the spatial dimension of the probe pulse, as well as resolving the spatial inhomogeneity contribution to the observed spectral broadening. Finally, after in situ exfoliation, we performed time-resolved μ-ARPES on a ∼30 μm flake of transition metal dichalcogenide WTe2, thus demonstrating the ability to access ultrafast electron dynamics with momentum resolution on micro-exfoliated materials. [ABSTRACT FROM AUTHOR]

The band structure and intra- and interband scattering processes of the electrons at the surface of a bismuth bilayer on Bi2Se3 have been experimentally investigated by low-temperature Fourier-transform scanning tunneling spectroscopy. The observed complex quasiparticle interference patterns are compared to a simulation based on the spin-dependent joint density of states approach using the surface-localized spectral function calculated from first principles as the only input. Thereby, the origin of the quasiparticle interferences can be traced back to intraband scattering in the bismuth-bilayer valence band and Bi2Se3 conduction band and to interband scattering between the two-dimensional topological state and the bismuth-bilayer valence band. The investigation reveals that the bilayer band gap, which is predicted to host one-dimensional topological states at the edges of the bilayer, is pushed several hundred meV above the Fermi level. This result is rationalized by an electron transfer from the bilayer to Bi2Se3 which also leads to a two-dimensional electron state in the Bi2Se3 conduction band with a strong Rashba spin splitting, coexisting with the topological state and bilayer valence band. [ABSTRACT FROM AUTHOR]

Homojunctions between Bi2Se3 and its Mn-doped phase are investigated as a sample geometry to study the influence of spin degrees of freedom on topological insulator properties. n quintuple layers of Bi2Se3 are grown on top of Mn-doped Bi2Se3 by molecular beam epitaxy for 0 ≤ n ≤ 30QLs, allowing to unhamperedly monitor the development of electronic and topological properties by surface sensitive techniques like angle resolved photoemission spectroscopy. With increasing n, a Mninduced gap at the Dirac point is gradually filled in an "hourglass" fashion to reestablish a topological surface state at n ∼ 9QLs. Our results suggest a competition of upward and downward band bending effects due to the presence of an n-p type interface, which can be used to tailor topological and quantum well states independently. [ABSTRACT FROM AUTHOR]

The article presents a study which explores the ubiquitous defect-induced density wave instability in monolayer graphene. It mentions the results reveal an unexpected sensitivity of the graphene lattice to dilute surface disorder and show that adsorbed atoms offer an attractive route toward designing novel phases in two-dimensional materials.

Ultrafast spectroscopies have become an important tool for elucidating the microscopic description and dynamical properties of quantum materials. In particular, by tracking the dynamics of nonthermal electrons, a material’s dominant scattering processes can be revealed. Here, we present a method for extracting the electron-phonon coupling strength in the time domain, using time-and angle-resolved photoemission spectroscopy (TR-ARPES). This method is demonstrated in graphite, where we investigate the dynamics of photoinjected electrons at the K point, detecting quantized energy-loss processes that correspond to the emission of strongly coupled optical phonons. We show that the observed characteristic time scale for spectral weight transfer mediated by phonon-scattering processes allows for the direct quantitative extraction of electron-phonon matrix elements for specific modes. [ABSTRACT FROM AUTHOR]

With its direct correspondence to electronic structure, angle-resolved photoemission spectroscopy (ARPES) is a ubiquitous tool for the study of solids. When extended to the temporal domain, time-resolved (TR)-ARPES offers the potential to move beyond equilibrium properties, exploring both the unoccupied electronic structure as well as its dynamical response under ultrafast perturbation. Historically, ultrafast extreme ultraviolet sources employing high-order harmonic generation (HHG) have required compromises that make it challenging to achieve a high energy resolution—which is highly desirable for many TR-ARPES studies—while producing high photon energies and a high photon flux. We address this challenge by performing HHG inside a femtosecond enhancement cavity, realizing a practical source for TR-ARPES that achieves a flux of over 1011 photons/s delivered to the sample, operates over a range of 8–40 eV with a repetition rate of 60 MHz. This source enables TR-ARPES studies with a temporal and energy resolution of 190 fs and 22 meV, respectively. To characterize the system, we perform ARPES measurements of polycrystalline Au and MoTe2, as well as TR-ARPES studies on graphite. [ABSTRACT FROM AUTHOR]

We report on the influence of spin-orbit coupling (SOC) in Fe-based superconductors via application of circularly polarized spin and angle-resolved photoemission spectroscopy. We combine this technique in representative members of both the Fe-pnictides (LiFeAs) and Fe-chalcogenides (FeSe) with tight-binding calculations to establish an ubiquitous modification of the electronic structure in these materials imbued by SOC. At low energy, the influence of SOC is found to be concentrated on the hole pockets, where the largest superconducting gaps are typically found. This effect varies substantively with the kz dispersion, and in FeSe we find SOC to be comparable to the energy scale of orbital order. These results contest descriptions of superconductivity in these materials in terms of pure spin-singlet eigenstates, raising questions regarding the possible pairing mechanisms and role of SOC therein. [ABSTRACT FROM AUTHOR]

Methods to generate spin-polarized electronic states in non-magnetic solids are strongly desired to enable all-electrical manipulation of electron spins for new quantum devices. This is generally accepted to require breaking global structural inversion symmetry. In contrast, here we report the observation from spin- and angle-resolved photoemission spectroscopy of spin-polarized bulk states in the centrosymmetric transition-metal dichalcogenide WSe2. Mediated by a lack of inversion symmetry in constituent structural units of the bulk crystal where the electronic states are localized, we show how spin splittings up to 0.5 eV result, with a spin texture that is strongly modulated in both real and momentum space. Through this, our study provides direct experimental evidence for a putative locking of the spin with the layer and valley pseudospins in transition-metal dichalcogenides, of key importance for using these compounds in proposed valleytronic devices. [ABSTRACT FROM AUTHOR]

Magnetotransport constitutes a useful probe to understand the interplay between electronic band topology and magnetism in spintronic devices. A recent theory of Lu and Shen [Phys. Rev. Lett. 112, 146601 (2014)] on magnetically doped topological insulators predicts that quantum corrections Δκ to the temperature dependence of conductivity can change sign across the Curie transition. This phenomenon has been attributed to a suppression of the Berry phase of the topological surface states at the Fermi level, caused by a magnetic energy gap. Here, we demonstrate experimentally that Δκ can reverse its sign even when the Berry phase at the Fermi level remains unchanged. The contradictory behavior to theory predictions is resolved by extending the model by Lu and Shen to a nonmonotonic temperature scaling of the inelastic scattering length showing a turning point at the Curie transition. [ABSTRACT FROM AUTHOR]

We report on the quenching of single Ni adatom moments on Te-terminated Bi2Te2Se and Bi2Te3 topological insulator surfaces. The effect is noted as a missing x-ray magnetic circular dichroism for resonant L3,2 transitions into partially filled Ni 3d states of theory-derived occupancy nd=9.2. On the basis of a comparative study of Ni and Fe using scanning tunneling microscopy and ab initio calculations, we are able to relate the element specific moment formation to a local Stoner criterion. Our theory shows that while Fe adatoms form large spin moments of ms=2.54μB with out-of-plane anisotropy due to a sufficiently large density of states at the Fermi energy, Ni remains well below an effective Stoner threshold for local moment formation. With the Fermi level remaining in the bulk band gap after adatom deposition, nonmagnetic Ni and preferentially out-of-plane oriented magnetic Fe with similar structural properties on Bi2Te2Se surfaces constitute a perfect platform to study the off-on effects of time-reversal symmetry breaking on topological surface states. [ABSTRACT FROM AUTHOR]