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Non-equilibrium conditions may lead to novel properties of materials with broken symmetry ground states not accessible in equilibrium as vividly demonstrated by non-linearly driven mid-infrared active phonon excitation. Potential energy surfaces of electronically excited states also allow to direct nuclear motion, but relaxation of the excess energy typically excites fluctuations leading to a reduced or even vanishing order parameter as characterized by an electronic energy gap. Here, using femtosecond time- and angle-resolved photoemission spectroscopy, we demonstrate a tendency towards transient stabilization of a charge density wave after near-infrared excitation, counteracting the suppression of order in the non-equilibrium state. Analysis of the dynamic electronic structure reveals a remaining energy gap in a highly excited transient state. Our observation can be explained by a competition between fluctuations in the electronically excited state, which tend to reduce order, and transiently enhanced Fermi surface nesting stabilizing the order., Whilst excited electronic states may exhibit unique non-equilibrium behavior, order is inhibited by fluctuations. Here, the authors use femtosecond photoemission spectroscopy to demonstrate transient stabilization of charge density wave order in rare earth tritellurides after near-infrared excitation.

We present a combined ultrafast optical pump-probe and ultrafast x-ray diffraction measurement of the CDW dynamics in SmTe$_3$ at 300 K. The ultrafast x-ray diffraction measurements, taken at the Linac Coherent Light Source reveal a $\sim 1.55$ THz mode that becomes overdamped with increasing fluence. We identify this oscillation with the lattice component of the amplitude mode. Furthermore, these data allow for a more clear identification of the frequencies present in the optical pump-probe data. In both, reflectivity and diffraction, we observe a crossover of the response from linear (for small displacements) to quadratic in the amplitude of the order parameter displacement. Finally, a time-dependent Ginzburg-Landau model captures the essential features of the experimental observations., Comment: 7 pages, 5 figures

We investigate the lattice coupling to the spin and charge orders in the striped nickelate, ${\mathrm{La}}_{1.75}{\mathrm{Sr}}_{0.25}{\mathrm{NiO}}_{4}$, using time-resolved resonant x-ray scattering. Lattice-driven dynamics of both spin and charge orders are observed when the pump photon energy is tuned to that of an ${E}_{u}$ bond- stretching phonon. We present a likely scenario for the behavior of the spin and charge order parameters and its implications using a Ginzburg-Landau theory.

We use ultrafast resonant x-ray diffraction to study the magnetic order in CuO under conditions of high electronic excitation. By measuring changes in the spectral shape of the Cu2+ magnetic (1/2 0 â1/2) reflection we investigate how an intense optical pump pulse perturbs the electronic and magnetic states. We observe an energy shift in the magnetic resonance at short times after the pump pulse. This shift is compared with expectations from band structure calculations at different electronic temperatures. This spectral line shift indicates that although the electrons are heated to effective electron temperatures far above TN on a time scale faster than the experimental resolution, magnetic order persists in this highly excited state for several hundred femtoseconds. © 2014 American Physical Society.

We study optimally doped Bi-2212 ($T_\textrm{c}=96$~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 one to two 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., Comment: 5 pages, 3 figures, accepted by Physical Review Letters

We characterize the topological insulator Bi$_2$Se$_3$ using time- and angle- resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second, Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained by a meta-stable population of the bulk conduction band. Finally, we perform a temperature-dependent study of the electron-phonon scattering processes in the conduction band, and find the unexpected result that their rates decrease with increasing sample temperature. We develop a model of phonon emission and absorption from a population of electrons, and show that this counter-intuitive trend is the natural consequence of fundamental electron-phonon scattering processes. This analysis serves as an important reminder that the decay rates extracted by time-resolved photoemission are not in general equal to single electron scattering rates, but include contributions from filling and emptying processes from a continuum of states., Comment: In Press: Journal of Electron Spectroscopy & Related Phenomena (special issue on 2-photon photoemission spectroscopy)

We perform time- and angle-resolved photoelectron spectroscopy on p-type GaAs(110). We observe an optically excited population in the conduction band, from which the time scales of intraband relaxation and surface photovoltage decay are both extracted. Moreover, the photovoltage shift of the valence band intriguingly persists for hundreds of picoseconds at negative delays. By comparing to a recent theoretical study, we reveal that the negative-delay dynamics reflects the interaction of the photoelectrons with a photovoltage-induced electric field outside the sample surface. We develop a conceptual framework to disentangle the intrinsic electron dynamics from this long-range field effect, which sets the foundation for understanding time-resolved photoemission experiments on a broad range of materials in which poor electronic screening leads to surface photovoltage. Finally, we demonstrate how the long-lasting negative-delay dynamics in GaAs can be utilized to conveniently establish the temporal overlap of pump and probe pulses in a time-resolved photoemission setup., Comment: 6 pages, 5 figures

© 2016 AIP Publishing LLC. We developed a table-top vacuum ultraviolet (VUV) laser with 113.778 nm wavelength (10.897 eV) and demonstrated its viability as a photon source for high resolution angle-resolved photoemission spectroscopy (ARPES). This sub-nanosecond pulsed VUV laser operates at a repetition rate of 10 MHz, provides a flux of 2 × 1012photons/s, and enables photoemission with energy and momentum resolutions better than 2 meV and 0.012 Å-1, respectively. Space-charge induced energy shifts and spectral broadenings can be reduced below 2 meV. The setup reaches electron momenta up to 1.2 Å-1, granting full access to the first Brillouin zone of most materials. Control over the linear polarization, repetition rate, and photon flux of the VUV source facilitates ARPES investigations of a broad range of quantum materials, bridging the application gap between contemporary low energy laser-based ARPES and synchrotron-based ARPES. We describe the principles and operational characteristics of this source and showcase its performance for rare earth metal tritellurides, high temperature cuprate superconductors, and iron-based superconductors.

Charge transfer pathways and charge transfer times in molecular films and in adsorbate layers depend both on the details of the electronic structure as well as on the degree of the initial localization of the propagating excited electronic state. For C6F6 molecular adsorbate films on the Cu(111) surface we determined the interplay between excited state localization and charge transfer pathways. In particular we selectively prepared a free-particle-like LUMO band excitation and compared it to a molecularly localized core-excited C1s -> pi* C6F6 LUMO state using time-resolved two-photon photoemission (tr-2PPE) and core-sole-clock (CHC) spectroscopy, respectively. For the molecularly localized core-excited C1s -> pi* C6F6 LUMO state, we separate the intramolecular dynamics from the charge transfer dynamics to the metal substrate by taking the intramolecular dynamics of the free C6F6 molecule into account Our analysis yields a generally applicable description of charge transfer within molecular adsorbates and to the substrate. (C) 2011 Published by Elsevier B.V.

Elementary scattering processes in solid matter occur on ultrafast timescales and photoelectron spectroscopy in the time domain represents an excellent tool for their analysis. Conventional photoemission accesses binding energies of electronic states and their momentum dispersion. The use of femtosecond laser pulses in pump-probe experiments allows obtaining direct insights to the energy and momentum dependence of ultrafast dynamics. This article introduces the elementary interaction processes and emphasizes recent work performed in this rapidly developing field. Decay processes in the low excitation limit are addressed, where electrons decay according to their interaction with carriers in equilibrium. Here, hot electron relaxation in epitaxial metallic film is reviewed. In the limit of an intense optical excitation, scattering of the excited electrons among each other establishes a non-equilibrium state. Results on charge-density wave materials and the effect of coherent nuclear motion on the electronic structure, which can break low symmetry ground states, are discussed. Figure reprinted with permission from [71].

We investigated ultrafast energy relaxation in unoccupied quantum well states of Pb/Si(111) with femtosecond time-resolved two-photon photoemission. Decay rates of 6pz quantum well states are compatible with Fermi liquid theory if inter-subband scattering is considered.

Ultrafast electron dynamics in Pb/Si(111) quantum well structures have been investigated by femtosecond time-resolved two-photon photoemission spectroscopy. Three unoccupied quantum well states (or subbands) as well as an image potential state are identified and analyzed as a function of Pb thickness. Using 1.9 eV photon energy for optical excitation electron-hole pairs are formed in the Pb film and in the Si substrate. The hot electron population in the quantum well states exhibits a biexponential decay and both decay times increase when the energy difference to the Fermi level is reduced. The slower decay component with decay times of 130 and 900 fs is attributed to delayed filling of the states in the adlayer due to electronic relaxation in the Si(111) substrate. The faster decay (30--140 fs) is caused by electron-electron scattering in the Pb film. At a first glance, the extracted decay times increase toward the Fermi level as predicted by the Fermi-liquid theory. However, by investigation of the quantized electronic structure more detailed insight into scattering among defined subbands has been gained. The rise of the excited electron population in the lowest unoccupied quantum well state is delayed by 70 fs which occurs concomitantly with a decay in the second lowest state. We describe this simultaneous decay and rise in the two adjacent subbands by coupled rate equations and attribute it to intersubband scattering. Thereby, we demonstrate the importance of intersubband decay in low-dimensional metallic systems in addition to intraband scattering processes considered in Fermi-liquid theory and derived descriptions.

We use laser-induced photoemission spectroscopy at $6\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$ photon energy to investigate quantum well states of epitaxial Pb films on Si(111) as function of film thickness. The binding energies of the quantum well states were found in good agreement with density-functional calculations for a freestanding Pb slab. An oscillation of the work function with a period of 2 ML was observed as a function of film thickness, which correlates well with the oscillatory electron density at the Fermi level determined from the photoemission spectra.

We present time- and angle-resolved photoemission spectroscopy measurements on the charge density wave system CeTe$_{3}$. Optical excitation transiently populates the unoccupied band structure and reveals a gap size of 2$\Delta$ = 0.59 eV. The occupied Te-5p band dispersion is coherently modified by three modes at $\Omega_{1}$ = 2.2 THz, $\Omega_{2}$ = 2.7 THz and $\Omega_{3}$ = 3 THz. All three modes lead to small rigid energy shifts whereas $\Delta$ is only affected by $\Omega_{1}$ and $\Omega_{2}$. Their spatial polarization is analyzed by fits of a transient model dispersion and DFT frozen phonon calculations. We conclude that the modes $\Omega_{1}$ and $\Omega_{2}$ result from in-plane ionic lattice motions, which modulate the charge order, and that $\Omega_{3}$ originates from a generic out-of-plane $A_{1g}$ phonon. We thereby demonstrate how the rich information from trARPES allows identification of collective modes and their spatial polarization, which explains the mode-dependent coupling to charge order., Comment: 5 pages, 4 figures

Comparing optical and core-hole excitation, we study relaxation dynamics of excited electrons at C6F6/Cu(111) interfaces. The pronounced tenfold difference in relaxation times is attributed to electron transfer across the interface and intra-molecular electron delocalization, respectively.

The advances in femtosecond laser techniques facilitate the investigation of ultrafast electron dynamics at surfaces directly in the time-domain. We employ time-resolved two-photon-photoemission (2PPE) spectroscopy to study the electron dynamics of the unoccupied electronic states in hexafluorobenzene (C6F6) on Cu(1 1 1) serving as a model system for charge transfer across organic–metal interfaces. Our coverage-dependent study reveals a lifetime of the lowest unoccupied molecular resonance of 7 fs for a single monolayer (ML) which increases to 37 fs above 3 ML coverage. We find that the population build-up of the excited state is delayed by a characteristic time of about 10 fs with respect to the exciting laser pulse. By angle-resolved 2PPE spectroscopy, the mechanism of the delayed population rise is identified as intraband relaxation in the adsorbate band structure. The actual electron-transfer to the metal substrate occurs through interband scattering between the molecular resonance and substrate states on comparable timescales. Therefore the present study demonstrates that relaxation of hot electrons at molecule–metal interfaces include—even in the presence of strong electronic molecule–substrate interaction—also decay channels within the adlayer.

Time- and angle-resolved photoelectron spectroscopy (trARPES) employing a 500 kHz extreme-ultravioled (XUV) light source operating at 21.7 eV probe photon energy is reported. Based on a high-power ytterbium laser, optical parametric chirped pulse amplification (OPCPA), and ultraviolet-driven high-harmonic generation, the light source produces an isolated high-harmonic with 110 meV bandwidth and a flux of more than $10^{11}$ photons/second 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., Comment: Accepted for publication in Review of Scientific Instruments