Search

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]

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]

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]