Dominik Leuenberger

Energy distribution curves of ultrafast laser-induced field emission and their implications for electron dynamics

Hirofumi Yanagisawa, Matthias Hengsberger, Dominik Leuenberger, Martin Klöckner, Christian Hafner, Thomas Greber, and Jürg Osterwalder Physik Institut, Universität Zürich, Winterthurerstrasse 190, CH-8057 Zürich, Switzerland Laboratory for Electromagnetic Fields and Microwave Electronics, ETH Zürich, Gloriastrasse 35, CH-8092 Zürich, Switzerland Present address: Department of Physics, ETH Zürich, Wolfgang-Pauli-Strasse 16, CH-8093 Zürich, Swizerland (Dated: January 15, 2013)

Optical control of field-emission sites by femtosecond laser pulses.

We have investigated field-emission patterns from a clean tungsten tip apex induced by femtosecond laser pulses. Strongly asymmetric modulations of the field-emission intensity distributions are observed depending on the polarization of the light and the laser incidence direction relative to the azimuthal orientation of tip apex. In effect, we have realized an ultrafast pulsed field-emission source with site selectivity. Simulations of local fields on the tip apex and of electron emission patterns based on photoexcited nonequilibrium electron distributions explain our observations quantitatively.

Laser-induced field emission from a tungsten tip: Optical control of emission sites and the emission process

Field-emission patterns from a clean tungsten tip apex induced by femtosecond laser pulses have been investigated. Strongly asymmetric field-emission intensity distributions are observed depending on three parameters: (i) the polarization of the light, (ii) the azimuthal, and (iii) the polar orientation of the tip apex relative to the laser incidence direction. In effect, we have realized an ultrafast pulsed field-emission source with site selectivity of a few tens of nanometers. Simulations of local fields on the tip apex and of electron emission patterns based on photoexcited nonequilibrium electron distributions explain our observations quantitatively. Electron emission processes are found to depend on laser power and tip voltage. At relatively low laser power and high tip voltage, field-emission after two-photon photoexcitation is the dominant process. At relatively low laser power and low tip voltage, photoemission processes are dominant. As the laser power increases, photoemission from the tip shank becomes noticeable. © 2010 The American Physical Society

Distinguishing Bulk and Surface Electron-Phonon Coupling in the Topological Insulator Bi 2 Se 3 Using Time-Resolved Photoemission Spectroscopy

We report time- and angle-resolved photoemission spectroscopy measurements on the topological insulator Bi(2)Se(3). We observe oscillatory modulations of the electronic structure of both the bulk and surface states at a frequency of 2.23 THz due to coherent excitation of an A(1g) phonon mode. A distinct, additional frequency of 2.05 THz is observed in the surface state only. The lower phonon frequency at the surface is attributed to the termination of the crystal and thus reduction of interlayer van der Waals forces, which serve as restorative forces for out-of-plane lattice distortions. Density functional theory calculations quantitatively reproduce the magnitude of the surface phonon softening. These results represent the first band-resolved evidence of the A(1g) phonon mode coupling to the surface state in a topological insulator.

Femtosecond electron-phonon lock-in by photoemission and x-ray free-electron laser

A deeper look into iron selenide In the past 10 years, iron-based superconductors have created more puzzles than they have helped resolve. Some of the most fundamental outstanding questions are how strong the interactions are and what the electron pairing mechanism is. Now two groups have made contributions toward resolving these questions in the intriguing compound iron selenide (FeSe) (see the Perspective by Lee). Gerber et al. used photoemission spectroscopy coupled with x-ray diffraction to find that FeSe has a very sizable electron-phonon interaction. Quasiparticle interference imaging helped Sprau et al. determine the shape of the superconducting gap and find that the electron pairing in FeSe is orbital-selective. Science, this issue p. 71, p. 75; see also p. 32 Photoemission spectroscopy coupled with x-ray diffraction reveals a sizable electron-phonon interaction in iron selenide. The interactions that lead to the emergence of superconductivity in iron-based materials remain a subject of debate. It has been suggested that electron-electron correlations enhance electron-phonon coupling in iron selenide (FeSe) and related pnictides, but direct experimental verification has been lacking. Here we show that the electron-phonon coupling strength in FeSe can be quantified by combining two time-domain experiments into a “coherent lock-in” measurement in the terahertz regime. X-ray diffraction tracks the light-induced femtosecond coherent lattice motion at a single phonon frequency, and photoemission monitors the subsequent coherent changes in the electronic band structure. Comparison with theory reveals a strong enhancement of the coupling strength in FeSe owing to correlation effects. Given that the electron-phonon coupling affects superconductivity exponentially, this enhancement highlights the importance of the cooperative interplay between electron-electron and electron-phonon interactions.

Inequivalence of Single-Particle and Population Lifetimes in a Cuprate Superconductor

We study optimally doped Bi-2212 (T(c)=96  K) using femtosecond time- and angle-resolved photoelectron spectroscopy. Energy-resolved population lifetimes are extracted and compared with single-particle lifetimes measured by equilibrium photoemission. The population lifetimes deviate from the single-particle lifetimes in the low excitation limit by 1-2 orders of magnitude. Fundamental considerations of electron scattering unveil that these two lifetimes are in general distinct, yet for systems with only electron-phonon scattering they should converge in the low-temperature, low-fluence limit. The qualitative disparity in our data, even in this limit, suggests that scattering channels beyond electron-phonon interactions play a significant role in the electron dynamics of cuprate superconductors.

Direct characterization of photoinduced lattice dynamics in BaFe2As2.

Ultrafast light pulses can modify electronic properties of quantum materials by perturbing the underlying, intertwined degrees of freedom. In particular, iron-based superconductors exhibit a strong coupling among electronic nematic fluctuations, spins and the lattice, serving as a playground for ultrafast manipulation. Here we use time-resolved X-ray scattering to measure the lattice dynamics of photoexcited BaFe2As2. On optical excitation, no signature of an ultrafast change of the crystal symmetry is observed, but the lattice oscillates rapidly in time due to the coherent excitation of an A1g mode that modulates the Fe–As–Fe bond angle. We directly quantify the coherent lattice dynamics and show that even a small photoinduced lattice distortion can induce notable changes in the electronic and magnetic properties. Our analysis implies that transient structural modification can be an effective tool for manipulating the electronic properties of multi-orbital systems, where electronic instabilities are sensitive to the orbital character of bands.

Excitation of Coherent Phonons in the One-Dimensional Bi(114) Surface

We present time-resolved photoemission experiments from a peculiar bismuth surface, Bi(114). The strong one-dimensional character of this surface is reflected in the Fermi surface, which consists of spin-polarized straight lines. Our results show that the depletion of the surface state and the population of the bulk conduction band after the initial optical excitation persist for very long times. The disequilibrium within the hot electron gas along with strong electron-phonon coupling cause a displacive excitation of coherent phonons, which in turn are reflected in coherent modulations of the electronic states. Beside the well-known A(1g) bulk phonon mode at 2.76 THz, the time-resolved photoelectron spectra reveal a second mode at 0.72 THz which can be attributed to an optical surface phonon mode along the atomic rows of the Bi(114) surface.

Thickness-Dependent Coherent Phonon Frequency in Ultrathin FeSe/SrTiO3 Films

Ultrathin FeSe films grown on SrTiO3 substrates are a recent milestone in atomic material engineering due to their important role in understanding unconventional superconductivity in Fe-based materials. By using femtosecond time- and angle-resolved photoelectron spectroscopy, we study phonon frequencies in ultrathin FeSe/SrTiO3 films grown by molecular beam epitaxy. After optical excitation, we observe periodic modulations of the photoelectron spectrum as a function of pump-probe delay for 1-unit-cell, 3-unit-cell, and 60-unit-cell thick FeSe films. The frequencies of the coherent intensity oscillations increase from 5.00 ± 0.02 to 5.25 ± 0.02 THz with increasing film thickness. By comparing with previous works, we attribute this mode to the Se A1g phonon. The dominant mechanism for the phonon softening in 1-unit-cell thick FeSe films is a substrate-induced lattice strain. Our results demonstrate an abrupt phonon renormalization due to a lattice mismatch between the ultrathin film and the substrate.

Classification of collective modes in a charge density wave by momentum-dependent modulation of the electronic band structure

We present time- and angle-resolved photoemission spectroscopy (trARPES) measurements on the charge density wave system CeTe3. Optical excitation transiently populates the unoccupied band structure and reveals a gap size of 2� = 0.59 eV. The occupied Te-5p band dispersion is coherently modified by three modes at