SIMES Publications

Abstract

Quantum-well states appear in metallic thin films due to the confinement of the wave function by the film interfaces. Using angle-resolved photoemission spectroscopy, we unexpectedly observe quantum-well states in fractured single crystals of CeCoIn₅. We confirm that confinement occurs by showing that these states’ binding energies are photon-energy independent and are well described with a phase accumulation model, commonly applied to quantum-well states in thin films. This indicates that atomically flat thin films can be formed by fracturing hard single crystals. For the two samples studied, our observations are explained by free-standing flakes with thicknesses of 206 and 101 Å. We extend our analysis to extract bulk properties of CeCoIn₅. Specifically, we obtain the dispersion of a three-dimensional band near the zone center along in-plane and out-of-plane momenta. We establish part of its Fermi surface, which corresponds to a hole pocket centered at Γ. We also reveal a change of its dispersion with temperature, a signature that may be caused by the Kondo hybridization.

Abstract

Time- and angle-resolved photoemission spectroscopy is a powerful probe of electronic band structures out of equilibrium. Tuning time and energy resolution to suit a particular scientific question has become an increasingly important experimental consideration. Many instruments use cascaded frequency doubling in nonlinear crystals to generate the required ultraviolet probe pulses. We demonstrate how calculations clarify the relationship between laser bandwidth and nonlinear crystal thickness contributing to experimental resolutions and place intrinsic limits on the achievable time-bandwidth product. Experimentally, we tune time and energy resolution by varying the thickness of nonlinear β-BaB₂O₄ crystals for frequency upconversion, providing a flexible experiment design. We achieve time resolutions of 58–103 fs and corresponding energy resolutions of 55–27 meV. We propose a method to select crystal thickness based on desired experimental resolutions.

Abstract

Experiments using a THz pump and an X-ray probe at an X-ray free-electron laser (XFEL) facility like the Linac Coherent Light Source II (LCLS II) require frequency-tunable (3 to 20 THz), narrow bandwidth (~10%), carrier-envelopephase-stable THz pulses that produce high fields (>1 MV cm^-1) at the repetition rate of the X-rays and are well synchronized with them. In this paper, a two-bunch scheme to generate THz radiation at LCLS II is studied: the first bunch produces THz radiation in an electromagnet wiggler immediately following the LCLS II undulator that produces X-rays from the second bunch. The initial time delay between the two bunches is optimized to compensate for the path difference in THz transport. The two-bunch beam dynamics, the THz wiggler and radiation are described, as well as the transport system bringing the THz pulses from the wiggler to the experimental hall.

Abstract

We determine the work functions of the iron arsenic compounds AFe₂As₂ (A=Ca,Ba,Cs) using photoemission spectroscopy to be 2.7 eV for CaFe₂As₂, 1.8 eV for BaFe₂As₂, and 1.3 eV for CsFe₂As₂. The work functions of these 122 iron-based superconductors track those of the elementary metal A but are substantially smaller. The most likely explanation of this observation is that the cleaving surface exposes only half an A-layer. The low work function and good photoemission cross section of BaFe₂As₂ and CsFe₂As₂ enable photoemission even from a common white LED light.

Abstract

We report the observation of efficient high-harmonic generation in the three-dimensional topological insulators Bi₂Se₃ and Bi₂Te₃ driven by mid-infrared laser pulses of peak intensities ~10¹² W/cm².

Abstract

Cuprate superconductors host a multitude of low-energy optical phonons. Using time- and angleresolved photoemission spectroscopy, we study coherent phonons inBi₂Sr₂Ca_0.92Y_0.08Cu₂O_8+δ. Sub-meV modulations of the electronic band structure are observed at frequencies of 3.94±0.01 and 5.59 ±0.06 THz. For the dominant mode at 3.94 THz, the amplitude of the band energy oscillation weakly increases as a function of momentum away from the node. Theoretical calculations allow identifying the observed modes as CuO₂-derived A_1g phonons. The Bi- and Sr-derived A_1g modes which dominate Raman spectra in the relevant frequency range are absent in our measurements. This highlights the mode selectivity for phonons coupled to the near-Fermi-level electrons, which originate from CuO₂ planes and dictate thermodynamic properties.

Abstract

We study the microscopic origins of photocurrent generation in the topological insulator ${\mathrm{Bi}}_2{\mathrm{Se}}_3$ via time- and angle-resolved photoemission spectroscopy. We image the unoccupied band structure as it evolves following a circularly polarized optical excitation and observe an asymmetric electron population in momentum space, which is the spectroscopic signature of a photocurrent. By analyzing the rise times of the population we identify which occupied and unoccupied electronic states are coupled by the optical excitation. We conclude that photocurrents can only be excited via resonant optical transitions coupling to spin-orbital textured states. Our work provides a microscopic understanding of how to control photocurrents in systems with spin-orbit coupling and broken inversion symmetry.

Abstract

We present ultrafast optical pump-probe and ultrafast x-ray diffraction measurements of the charge density wave dynamics in SmTe₃ at 300 K. We performed ultrafast x-ray diffraction measurements at the Linac Coherent Light Source to directly probe the dynamics of the finite-wave-vector order parameter. The dynamics reveal coherent oscillations at ∼1.6 THz that become overdamped with increasing fluence. We identify this oscillation with the lattice component of the amplitude mode. Furthermore, our data allow for a clear identification of the amplitude mode frequency in the optical pump-probe data. In both measurements, the system reaches the symmetric phase at high fluence, where the order parameter vanishes and the response (reflectivity and x-ray intensity) is quadratic in the order parameter. This is observed in the x-ray diffraction as a small overdamped modulation near zero intensity. Similar overdamped features are observed in the optical reflectivity at high fluence. A time-dependent Ginzburg-Landau model captures qualitatively the essential features of the experimental observations.

Abstract

Time- and angle-resolved photoemission spectroscopy (trARPES) employing a 500 kHz extreme-ultraviolet light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification, and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than 10¹¹ photons/s on the sample. Combined with a state-of-the-art ARPES chamber, this table-top experiment allows high-repetition rate pump-probe experiments of electron dynamics in occupied and normally unoccupied (excited) states in the entire Brillouin zone and with a temporal system response function below 40 fs.

Abstract

Research in topological matter has expanded to include the Dirac and Weyl semimetals1,2,3,4,5,6,7,8,9,10, which feature three-dimensional Dirac states protected by symmetry. Zirconium pentatelluride has been of recent interest as a potential Dirac or Weyl semimetal material. Here, we report the results of experiments performed by in situ three-dimensional double-axis rotation to extract the full 4π solid angular dependence of the transport properties. A clear anomalous Hall effect is detected in every sample studied, with no magnetic ordering observed in the system to the experimental sensitivity of torque magnetometry. Large anomalous Hall signals develop when the magnetic field is rotated in the plane of the stacked quasi-two-dimensional layers, with the values vanishing above about 60 K, where the negative longitudinal magnetoresistance also disappears. This suggests a close relation in their origins, which we attribute to the Berry curvature generated by the Weyl nodes.