Halogen bonding has recently been recognized as an interaction whose relevance is on par with hydrogen bonding. While observed frequently in solution chemistry, the significance of halogen bonds in forming extended supramolecular structures on surfaces is less explored. Herein, we report on the self-assembly of chlorobenzene molecules adsorbed on the Cu(111) surface into nanosized clusters at submonolayer coverages, where the molecular planes are close to parallel to the surface. A comprehensive study of the role of intermolecular interactions through both halogen and weak hydrogen bonds on nanocluster formation is presented, gained by combining the results of temperature-programmed desorption, reflection-absorption infrared spectroscopy, scanning tunneling microscopy, and density functional theory calculations. Based on an unprecedented precise determination of the molecules’ orientation within the clusters, the binding motifs that lead to the formation and stability of nanoclusters with magic sizes are identified and explained. A complex and delicate interplay of halogen bonds with weak hydrogen bonds, van-der-Waals forces, and surface–adsorbate interactions leads to a preference for hexamers and tetramers with an observable propensity for halogen bonding over weak hydrogen bonding when adsorbed to the Cu(111) surface. © 2021 American Chemical Society

Microscopic insight into interactions is a key for understanding the properties of heterogenous interfaces. We analyze local attraction in noncovalently bonded Xe-Cs+ aggregates and monolayers on Cu(111) as well as repulsion upon electron transfer. Using two-photon photoemission spectroscopy, scanning tunneling microscopy, and coupled cluster calculations combined with an image-charge model, we explain the intricate impact Xe has on Cs+/Cu(111). We find that attraction between Cs+ and Xe counterbalances the screened Coulomb repulsion between Cs+ ions on Cu(111). Furthermore, we observe that the Cs 6s electron is repelled from Cu(111) due to xenon's electron density. Together, this yields a dual, i.e., attractive or repulsive, response of Xe depending on the positive or negative charge of the respective counterparticle, which emphasizes the importance of the Coulomb interaction in these systems. © 2021 American Physical Society.

Time-dependent and constituent-specific spectral changes in soft near-edge x-ray absorption spectroscopy (XAS) of an metal/insulator heterostructure after laser excitation are analyzed at the O K-edge with picosecond time resolution. The oxygen absorption edge of the insulator features a uniform intensity decrease of the fine structure at elevated phononic temperatures, which can be quantified by a simple simulation and fitting procedure presented here. Combining XAS with ultrafast electron diffraction measurements and ab initio calculations demonstrates that the transient intensity changes in XAS can be assigned to a transient lattice temperature. Thus, the sensitivity of transient near-edge XAS to phonons is demonstrated. © 2021 American Physical Society

Electron attachment and solvation at ice structures are well-known phenomena. The energy liberated in such events is commonly understood to cause temporary changes at such ice structures, but it may also trigger permanent modifications to a yet unknown extent. We determine the impact of electron solvation on D2O structures adsorbed on Cu(111) with low-Temperature scanning tunneling microscopy, two-photon photoemission, and ab initio theory. Solvated electrons, generated by ultraviolet photons, lead not only to transient but also to permanent structural changes through the rearrangement of individual molecules. The persistent changes occur near sites with a high density of dangling OD groups that facilitate electron solvation. We conclude that energy dissipation during solvation triggers permanent molecular rearrangement via vibrational excitation. Copyright © 2020 American Chemical Society.

Employing femtosecond laser pulses in front and back side pumping of Au/Fe/MgO(001) combined with detection in two-photon photoelectron emission spectroscopy, we analyze local relaxation dynamics of excited electrons in buried Fe, injection into Au across the Fe-Au interface, and electron transport across the Au layer at 0.6 to 2.0 eV above the Fermi energy. By analysis as a function of Au film thickness we obtain the electron lifetimes of bulk Au and Fe and distinguish the relaxation in the heterostructure's constituents. We also show that the excited electrons propagate through Au in a superdiffusive regime and conclude further that electron injection across the epitaxial interface proceeds ballistically by electron wave packet propagation. © 2020 American Physical Society.

By combining interface-sensitive nonlinear magneto-optical experiments with femtosecond time resolution and ab initio time-dependent density functional theory, we show that optically excited spin dynamics at Co/Cu(001) interfaces proceeds via spin-dependent charge transfer and back transfer between Co and Cu. This ultrafast spin transfer competes with dissipation of spin angular momentum mediated by spin-orbit coupling already on sub 100 fs timescales. We thereby identify the fundamental microscopic processes during laser-induced spin transfer at a model interface for technologically relevant ferromagnetic heterostructures. © 2019 American Physical Society.

Ultrafast reflection high-energy electron diffraction is employed to follow the lattice excitation of a Bi(111) surface upon irradiation with a femtosecond laser pulse. The thermal motion of the atoms is analyzed through the Debye-Waller effect. While the Bi bulk is heated on time scales of 2 to 4 ps, we observe that the excitation of vibrational motion of the surface atoms occurs much slower with a time constant of 12 ps. This transient nonequilibrium situation is attributed to the weak coupling between bulk and surface phonon modes which hampers the energy flow between the two subsystems. From the absence of a fast component in the transient diffraction intensity, it is in addition concluded that truncated bulk phonon modes are absent at the surface. © 2019 Author(s).

We demonstrate a novel method for the excitation of sizable magneto-optical effects in Au by means of the laser-induced injection of hot spin-polarized electrons in Au/Fe/MgO(0 0 1) heterostructures. It is based on the energy- and spin-dependent electron transmittance of Fe/Au interface which acts as a spin filter for non-thermalized electrons optically excited in Fe. We show that after crossing the interface, majority electrons propagate through the Au layer with the velocity on the order of 1 nm fs-1 (close to the Fermi velocity) and the decay length on the order of 100 nm. Featuring ultrafast functionality and requiring no strong external magnetic fields, spin injection results in a distinct magneto-optical response of Au. We develop a formalism based on the phase of the transient complex MOKE response and demonstrate its robustness in a plethora of experimental and theoretical MOKE studies on Au, including our ab initio calculations. Our work introduces a flexible tool to manipulate magneto-optical properties of metals on the femtosecond timescale that holds high potential for active magneto-photonics, plasmonics, and spintronics.

The element specificity of soft X-ray spectroscopy makes it an ideal tool for analyzing the microscopic origin of ultrafast dynamics induced by localized optical excitation in metal-insulator heterostructures. Using [Fe/MgO]n as a model system, we perform ultraviolet pump/soft X-ray probe experiments, which are sensitive to all constituents of these heterostructures, to probe both electronic and lattice excitations. Complementary ultrafast electron diffraction experiments independently analyze the lattice dynamics of the Fe constituent, and together with ab initio calculations yield comprehensive insight into the microscopic processes leading to local relaxation within a single constituent or nonlocal relaxation between two constituents. Besides electronic excitations in Fe, which are monitored at the Fe L3 absorption edge and relax within 1 ps by electron-phonon coupling, soft X-ray analysis identifies a change at the oxygen K absorption edge of the MgO layers which occurs within 0.5 ps. This ultrafast energy transfer across the Fe-MgO interface is mediated by high-frequency, interface vibrational modes, which are excited by hot electrons in Fe and couple to vibrations in MgO in a mode-selective, nonthermal manner. A second, slower timescale is identified at the oxygen K pre-edge and the Fe L3 edge. The slower process represents energy transfer by acoustic phonons and contributes to thermalization of the entire heterostructure. We thus find that the interfacial energy transfer is associated with nonequilibrium behavior in the phonon system. Because our experiments lack signatures of charge transfer across the interface, we conclude that phonon-mediated processes dominate the competition of electronic and lattice excitations in these nonlocal, nonequilibrium dynamics. © 2019 American Physical Society.

The high-Tc superconducting cuprates are recognized as doped Mott insulators. Several studies indicate that as a function of doping and temperature, there is a crossover from this regime into a phase characterized as a marginal Fermi liquid. Several calculations of the doped Mott insulating phase indicate that the Fermi surface defines small pockets which at the higher doping levels switch to a full closed Fermi surface, characteristic of a more metallic system. Here we use femtosecond laser-based pump-probe techniques to investigate the structure of the Fermi surface in the underdoped region of Bi2Sr2CaCu2O8+δ and compare it with that associated with the optimally doped material. We confirm the concept of a small pocket in the underdoped system consistent with theoretical predictions in this strongly correlated state. © 2019 American Physical Society.

Harmonic generation from solid surfaces is a promising tool for producing high-energy attosecond pulses. We report shaping of the harmonic spectrum to achieve the bandwidth necessary for attosecond pulse generation. The shaping is demonstrated for lower as well as for higher harmonics using single and two-pulse pumping. The measured harmonic field autocorrelation function exhibits attosecond spikes in good agreement with the harmonic spectrum. Double slit experiments reveal a high spatial coherence of the harmonic beam. © 2019 American Physical Society.

High-energy femtosecond laser pulses in the mid-infrared (MIR) wavelength range are essential for a wide range of applications from strong-field physics to selectively pump and probe low energy excitations in condensed matter and molecular vibrations. Here we report a four stage optical parametric chirped pulse amplifier (OPCPA) which generates ultrashort pulses at a central wavelength of 3000 nm with 430 µJ energy per pulse at a bandwidth of 490 nm. Broadband emission of a Ti:sapphire oscillator seeds both the four stage OPCPA 800 nm and the pump line at 1030 nm. The first stage amplifies the 800 nm pulses in BBO using a non-collinear configuration. The second stage converts the wavelength to 1560 nm using difference frequency generation in BBO in a collinear geometry. The third stage amplifies this frequency non-collinearly in KTA. Finally, the fourth stage generates the 3000 nm radiation in a collinear configuration in LiIO3 due to the broad amplification bandwidth this crystal provides. We compress these pulses to 65 fs by transmission through sapphire. Quantitative calculations of the individual non-linear processes in all stages verify that our OPCPA architecture operates close to optimum efficiency. Low absorption losses suggest that this particular design is very suitable for operation at high average power and multi kHz repetition rates. © 2019 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

The lattice response of a Bi(111) surface upon impulsive femtosecond laser excitation is studied with time-resolved reflection high-energy electron diffraction. We employ a Debye-Waller analysis at large momentum transfer of 9.3 Å -1 ≤ Δ k ≤ 21.8 Å -1 in order to study the lattice excitation dynamics of the Bi surface under conditions of weak optical excitation up to 2 mJ/cm 2 incident pump fluence. The observed time constants τ int of decay of diffraction spot intensity depend on the momentum transfer Δk and range from 5 to 12 ps. This large variation of τ int is caused by the nonlinearity of the exponential function in the Debye-Waller factor and has to be taken into account for an intensity drop ΔI > 0.2. An analysis of more than 20 diffraction spots with a large variation in Δk gave a consistent value for the time constant τ T of vibrational excitation of the surface lattice of 12 ± 1 ps independent on the excitation density. We found no evidence for a deviation from an isotropic Debye-Waller effect and conclude that the primary laser excitation leads to thermal lattice excitation, i.e., heating of the Bi surface. © 2019 Author(s).

We investigate the perturbation and subsequent recovery of the correlated electronic ground state of the Mott insulator 1T-TaS2 by means of femtosecond time-resolved photoemission spectroscopy in normal emission geometry. Upon an increase of near-infrared excitation strength, a considerable collapse of the occupied Hubbard band is observed, which reflects a quench of short-range correlations. It is furthermore found that these excitations are directly linked to the lifting of the periodic lattice distortion which provides the localization centers for the formation of the insulating Mott state. We discuss the observed dynamics in a localized real-space picture. © 2018 by the authors.

We use scanning tunneling microscopy, photoelectron spectroscopy, and ab initio calculations to investigate the electron-induced dissociation of halogenated benzene molecules adsorbed on ice. Dissociation of halobenzene is triggered by delocalized excess electrons attaching to the π∗ orbitals of the halobenzenes from where they are transferred to σ∗ orbitals. The latter orbitals provide a dissociative potential surface. Adsorption on ice sufficiently lowers the energy barrier for the transfer between the orbitals to facilitate dissociation of bromo- and chloro- but not of flourobenzene at cryogenic temperatures. Our results shed light on the influence of environmentally important ice particles on the reactivity of halogenated aromatic molecules. © 2018 American Physical Society.

The interplay between the electronic and lattice degrees of freedom in nonequilibrium states of strongly correlated systems has been debated for decades. Although progress has been made in establishing a hierarchy of electronic interactions with the use of time-resolved techniques, the role of the phonons often remains in dispute, a situation highlighting the need for tools that directly probe the lattice. We present the first combined megaelectron volt ultrafast electron diffraction and time- and angle-resolved photoemission spectroscopy study of optimally doped Bi2Sr2CaCu2O8+d. Quantitative analysis of the lattice and electron subsystems’ dynamics provides a unified picture of nonequilibrium electron-phonon interactions in the cuprates beyond the N-temperature model. The work provides new insights on the specific phonon branches involved in the nonequilibrium heat dissipation from the high-energy Cu–O bond stretching “hot” phonons to the lowest-energy acoustic phonons with correlated atomic motion along the <110> crystal directions and their characteristic time scales. It reveals a highly nonthermal phonon population during the first several picoseconds after the photoexcitation. The approach, taking advantage of the distinct nature of electrons and photons as probes, is applicable for studying energy relaxation in other strongly correlated electron systems. Copyright © 2018 The Authors.

Strongly correlated materials exhibit intriguing properties caused by intertwined microscopic interactions that are hard to disentangle in equilibrium. Employing nonequilibrium time-resolved photoemission spectroscopy on the quasi-two-dimensional transition-metal dichalcogenide 1T-TaS2, we identify a spectroscopic signature of doubly occupied sites (doublons) that reflects fundamental Mott physics. Doublon-hole recombination is estimated to occur on timescales of electronic hopping /J≈14 fs. Despite strong electron-phonon coupling, the dynamics can be explained by purely electronic effects captured by the single-band Hubbard model under the assumption of weak hole doping, in agreement with our static sample characterization. This sensitive interplay of static doping and vicinity to the metal-insulator transition suggests a way to modify doublon relaxation on the few-femtosecond timescale. © 2018 American Physical Society.

We discuss fundamental aspects of laser-induced ultrafast demagnetization probed by the time-resolved magneto-optical Kerr effect (MOKE). Studying thin Fe films on MgO substrate in the absence of electronic transport, we demonstrate how to disentangle pump-induced variations of magnetization and magneto-optical coefficients. We provide a mathematical formalism for retrieving genuine laser-induced magnetization dynamics and discuss its applicability in real experimental situations. We further stress the importance of temporal resolution achieved in the experiments and argue that measurements of both time-resolved MOKE rotation and ellipticity are needed for the correct assessment of magnetization dynamics on sub-picosecond timescales. The framework developed here sheds light onto the details of the time-resolved MOKE technique and contributes to the understanding of the interplay between ultrafast laser-induced optical and magnetic effects. © 2017 IOP Publishing Ltd.

In this article, we review our angle- and time-resolved photoemission studies (ARPES and trARPES) on various ferropnictides. In the ARPES studies, we focus first on the band structure as a function of control parameters. We find near optimally “doped” compounds a Lifshitz transition of hole/electron pocket vanishing type. Second, we investigated the inelastic scattering rates as a function of the control parameter. In contrast to the heavily discussed quantum critical scenario, we find no enhancement of the scattering rate near optimally “doping.” Correlation effects which show up by the non-Fermi-liquid behavior of the scattering rates, together with the Lifshitz transition offer a new explanation for the strange normal state properties and suggests an interpolating superconducting state between BCS and BE condensation. Adding femtosecond time resolution to ARPES provides complementary information on electron and lattice dynamics. We report on the response of the chemical potential by a collective periodic variation coupled to coherent optical phonons in combination with incoherent electron and phonon dynamics described by a three temperature heat bath model. We quantify electron phonon coupling in terms of λ 〈ω〉2 and show that the analysis of the electron excess energy relaxation is a robust approach. The spin density wave ordering leads to a pronounced momentum dependent relaxation dynamics. In the vicinity of kf, hot electrons dissipate their energy by electron–phonon coupling with a characteristic time constant of 200 fs. Electrons at the center of the hole pocket exhibit a four time slower relaxation which is explained by spin-dependent dynamics with its smaller relaxation phase space. This finding has implications beyond the material class of Fe-pnictides because it establishes experimental access to spin-dependent dynamics in materials with spin density waves. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Using the sensitivity of optical second harmonic generation to currents, we demonstrate the generation of 250-fs long spin current pulses in Fe/Au/Fe/MgO(001) spin valves. The temporal profile of these pulses indicates ballistic transport of hot electrons across a sub-100 nm Au layer. The pulse duration is primarily determined by the thermalization time of laser-excited hot carriers in Fe. Considering the calculated spin-dependent Fe/Au interface transmittance we conclude that a nonthermal spin-dependent Seebeck effect is responsible for the generation of ultrashort spin current pulses. The demonstrated rotation of spin polarization of hot electrons upon interaction with noncollinear magnetization at Au/Fe interfaces holds high potential for future spintronic devices. © 2017 American Physical Society.

We study the Fermi-Hubbard model in the strongly correlated Mott phase under the influence of a harmonically oscillating hopping rate J(t)=J0+ΔJcos(ωt). Apart from the well-known fundamental resonance, where the frequency ω of this oscillation equals (or a little exceeds) the Mott gap, we also find higher-order resonances where multiple particle-hole pairs are created when ω is near an integer multiple of the gap. These findings should be relevant for experimental realizations such as ultracold fermionic atoms in optical lattices or pump-probe experiments using laser pulses incident on correlated electrons in solid-state materials. © 2017 American Physical Society.

Spintronics had a widespread impact over the past decades due to transferring information by spin rather than electric currents. Its further development requires miniaturization and reduction of characteristic timescales of spin dynamics combining the sub-nanometre spatial and femtosecond temporal ranges. These demands shift the focus of interest towards the fundamental open question of the interaction of femtosecond spin current (SC) pulses with a ferromagnet (FM). The spatio-temporal properties of the impulsive spin transfer torque exerted by ultrashort SC pulses on the FM open the time domain for probing non-uniform magnetization dynamics. Here we employ laser-generated ultrashort SC pulses for driving ultrafast spin dynamics in FM and analysing its transient local source. Transverse spins injected into FM excite inhomogeneous high-frequency spin dynamics up to 0.6 THz, indicating that the perturbation of the FM magnetization is confined to 2 nm. © The Author(s) 2017.

Transient control over the atomic potential-energy landscapes of solids could lead to new states of matter and to quantum control of nuclear motion on the timescale of lattice vibrations. Recently developed ultrafast time-resolved diffraction techniques combine ultrafast temporal manipulation with atomic-scale spatial resolution and femtosecond temporal resolution. These advances have enabled investigations of photo-induced structural changes in bulk solids that often occur on timescales as short as a few hundred femtoseconds. In contrast, experiments at surfaces and on single atomic layers such as graphene report timescales of structural changes that are orders of magnitude longer. This raises the question of whether the structural response of low-dimensional materials to femtosecond laser excitation is, in general, limited. Here we show that a photo-induced transition from the low- to high-symmetry state of a charge density wave in atomic indium (In) wires supported by a silicon (Si) surface takes place within 350 femtoseconds. The optical excitation breaks and creates In-In bonds, leading to the non-thermal excitation of soft phonon modes, and drives the structural transition in the limit of critically damped nuclear motion through coupling of these soft phonon modes to a manifold of surface and interface phonons that arise from the symmetry breaking at the silicon surface. This finding demonstrates that carefully tuned electronic excitations can create non-equilibrium potential energy surfaces that drive structural dynamics at interfaces in the quantum limit (that is, in a regime in which the nuclear motion is directed and deterministic). This technique could potentially be used to tune the dynamic response of a solid to optical excitation, and has widespread potential application, for example in ultrafast detectors. © 2017 Macmillan Publishers Limited, part of Springer Nature. All rights reserved.

We analyze laser-induced ultrafast, spatially inhomogeneous magnetization dynamics of epitaxial Co/Cu(001) films in a 0.4-10 nm thickness range with time-resolved magnetization-induced second harmonic generation, which probes femtosecond spin dynamics at the vacuum/Co and Co/Cu interfaces. The interference of these two contributions makes the overall signal particularly sensitive to differences in the transient magnetization redistribution between the two interfaces, i.e., ultrafast magnetization profiles in the ferromagnetic film. We conclude that the magnetization dynamics within the first several hundred femtoseconds is characteristically dependent on the Co film thickness. In films up to 3 nm thickness, we find a stronger demagnetization at the film surface compared to the Cu/Co interface, which we explain by a spin current from Co into the Cu substrate with an effective mean free path of about 3 nm. For film thicknesses larger than 3 nm, the transient magnetization profile over the Co film reverses its sign since spins can be transferred into the substrate only from the interface near region. Our work emphasizes that spatial inhomogeneities in the dynamic magnetic response to femtosecond laser excitation allow conclusions on the underlying microscopic processes. © 2017 Author(s).

A previous time-resolved optical study reported on a metastable hidden electronic state in 1T-TaS2, which is only accessible upon photoexcitation and created under non-equilibrium conditions [1]. The properties of such a state are distinct from those of any other state in the equilibrium phase diagram and it is possible to revert to the thermodynamic initial state either by illuminating with picosecond laser pulses or by applying other thermal erase procedures. In this work we show photoinduced switching to a metastable hidden state on the same material, and probe it by means of both static and time-resolved photoemission spectroscopy, thus having direct access to the electronic structure of the system. From our experimental findings and comparison with other studies, we conclude that we obtain partial switching, leading to a hidden state with persisting insulating nature but significant modifications in the electronic structure and CDW ordering. © 2016 SPIE.

Ultrafast demagnetization after femtosecond laser excitation of thin ferromagnetic films has been shown to occur due to a combination of spin-flip scattering in the film and spin transport to a conducting substrate or adjacent layer. Here we demonstrate that the inherent depth sensitivity of the transversal magneto-optical Kerr effect can be employed to derive conclusions on a transient spatial profile in the magnetization in the direction normal to the sample surface. This magnetization profile is qualitatively different for demagnetization caused by spin flips and spin transport. With the help of simulations based on simple phenomenological models we show that spin transport to the substrate in Co/Cu(001) films dominates the demagnetization before the thermalization of the electronic system, i.e. at times < 100 fs, while after approximately 200 fs mainly spin-flip scattering determines the magnetization profile, in agreement with our earlier findings employing the longitudinal magneto-optical Kerr effect. © 2016 SPIE.

Using femtosecond time- and angle-resolved photoemission spectroscopy we investigate the effect of electron doping on the electron dynamics in Ba(Fe1-xCox)2As2 in a range of 0 ≤ x < 0.15 at temperatures slightly above the Nel temperature. By analyzing the time-dependent photoemission intensity of the pump laser excited population as a function of energy, we found that the relaxation times at 0 < E - EF < 0.2 eV are doping dependent and about 100 fs shorter at optimal doping than for overdoped and parent compounds. Analysis of the relaxation rates also reveals the presence of a pump fluence dependent step in the relaxation time at E - EF = 200 meV whichwe explain by coupling of the excited electronic system to a boson of this energy.Wecompare our results with static ARPES and transport measurements and find disagreement and agreement concerning the doping dependence, respectively. We discuss the effect of the electron-boson coupling on the energy dependent relaxation and assign the origin of the boson to a magnetic excitation.

In complex materials various interactions have important roles in determining electronic properties. Angle-resolved photoelectron spectroscopy (ARPES) is used to study these processes by resolving the complex single-particle self-energy and quantifying how quantum interactions modify bare electronic states. However, ambiguities in the measurement of the real part of the self-energy and an intrinsic inability to disentangle various contributions to the imaginary part of the self-energy can leave the implications of such measurements open to debate. Here we employ a combined theoretical and experimental treatment of femtosecond time-resolved ARPES (tr-ARPES) show how population dynamics measured using tr-ARPES can be used to separate electron-boson interactions from electron-electron interactions. We demonstrate a quantitative analysis of a well-defined electron-boson interaction in the unoccupied spectrum of the cuprate Bi 2 Sr 2 CaCu 2 O 8+x characterized by an excited population decay time that maps directly to a discrete component of the equilibrium self-energy not readily isolated by static ARPES experiments.

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. © 2016, Nature Publishing Group. All rights reserved.

Angle-resolved photoemission spectroscopy is used to study the band dispersion and the quasiparticle scattering rates in two ferropnictide systems. We find the scattering rate for any given band to depend linearly on energy but to be independent of the control parameter. We demonstrate that the linear energy dependence gives rise to a weakly dispersing band with a strong mass enhancement when the band maximum crosses the chemical potential. The resulting small effective Fermi energy favors a BCS [J. Bardeen, Phys. Rev. 108, 1175 (1957)PHRVAO0031-899X10.1103/PhysRev.108.1175] -Bose-Einstein [S. N. Bose, Z. Phys. 26, 178 (1924)EPJAFV1434-600110.1007/BF01327326] crossover state in the superconducting phase. © 2015 American Physical Society.

Ultrafast magnetization dynamics in metallic heterostructures consists of a combination of local demagnetization in the ferromagnetic constituent and spin-dependent transport contributions within and in between the constituents. Separation of these local and nonlocal contributions is essential to obtain microscopic understanding and for potential applications of the underlying microscopic processes. By comparing the ultrafast changes of the polarization rotation and ellipticity in the magneto-optical Kerr effect we observe a time-dependent magnetization profile M(z,t) in Co/Cu(001) films by exploiting the effective depth sensitivity of the method. By analyzing the spatiotemporal correlation of these profiles we find that on time scales before hot electron thermalization (<100 fs) the transient magnetization of Co films is governed by spin-dependent transport effects, while after hot electron thermalization (>200 fs) local spin-flip processes dominate. © 2015 American Physical Society.

Here we report on the ultrafast electron dynamics of the alkalis Na, K, and Cs coadsorbed with D2O on Cu(111) surfaces, which we investigated with femtosecond time-resolved two-photon photoemission. The well known transient electronic binding energy stabilization in bare adsorbed alkalis is enhanced by the presence of water which acts as a solvent and increases the transient energy gain. We observe for all adsorbed alkalis a transient binding energy stabilization of 100-300 meV. The stabilization rates range from 1 to 2 eV ps-1. Here the heavier alkali exhibits a slower stabilization which we explain by their weaker static alkali-water interaction observed in thermal desorption spectroscopy. The population dynamics at low water coverage is described by a single exponential. With increasing water coverage the behavior becomes non-exponential suggesting an additional excited state due to electron solvation. This journal is © the Owner Societies 2015.

Propagation dynamics of spin-dependent optical excitations is investigated by back-pump front-probe experiments in Au/Fe/Mg0(001). We observe a decrease for all pump-probe signals detected at the Au surface, if the Fe thickness in increased. Relaxation processes within Fe limit the emission region of ballistic spins at the Fe/Au interface to ∼1 nm. © Springer International Publishing Switzerland 2015.

We make a step towards the understanding of spin dynamics induced by spin-polarized hot carriers in metals. Exciting the Fe layer of Au/Fe/MgO(001) structures with femtosecond laser pulses, we demonstrate the ultrafast spin transport from Fe into Au using time-resolved MOKE and mSHG for depthsensitive detection of the transient magnetization. © Springer International Publishing Switzerland 2015.

The unoccupied electronic structure of quasi-one-dimensional reconstructions of Pb atoms on a Si(557) surface is investigated by means of femtosecond time- and angle-resolved two-photon photoemission. Two distinct unoccupied electronic states are observed at E-EF=3.55 and 3.30 eV, respectively. Density functional theory calculations reveal that these states are spatially located predominantly on the lead wires and that they are energetically degenerated with an energy window of reduced electronic density of states in Si. We further find momentum-averaged lifetimes of 24 and 35 fs of these two states, respectively. The photoemission yield and the population dynamics depend on the electron momentum component perpendicular to the steps of the Si substrate, and the momentum-dependent dynamics cannot be described by means of rate equations. We conclude that momentum- and direction-dependent dephasing of the electronic excitations, likely caused by elastic scattering at the step edges on the vicinal surface, modifies the excited-state population dynamics in this system. © 2015 American Physical Society.

The dynamics of the transient electronic structure in the charge density wave (CDW) system RTe3 (R = rare-earth element) is studied using time- and angle-resolved photoemission spectroscopy (trARPES). Employing a three-pulse pump-probe scheme we investigate the effect of the amplitude mode oscillations on the electronic band structure and, in particular, on the CDW energy gap. We observe coherent oscillations in both lower and upper CDW band with opposite phases, whereby two dominating frequencies are modulating the CDW order parameter. This demonstrates the existence of more than one collective amplitude mode, in contrast to a simple Peierls model. Coherent control experiments of the two amplitude modes, which are strongly coupled in equilibrium, demonstrate independent control of the modes suggesting a decoupling of both modes in the transient photoexcited state. © The Royal Society of Chemistry 2014.

From measurements of the transient Debye-Waller effect in Bismuth, we determine the buildup time of the random atomic motion resulting from the electronic relaxation after short pulse laser excitation. The surface sensitive reflection high energy electron diffraction and transmission electron diffraction yield a time constant of about 12 ps and 3 ps, respectively. The different energy transfer rates indicate relatively weak coupling between bulk and surface vibrational modes. © 2014 AIP Publishing LLC.

The electron-phonon coupling parameters in the vicinity of the γ̄ point, λ(γ̄), for electronic quantum well states in epitaxial lead films on a Si(1 1 1) substrate are measured using 5, 7 and 12ML films and femtosecond laser photoemission spectroscopy. The λ (γ̄) values in the range of 0.6-0.9 were obtained by temperature-dependent line width analysis of occupied quantum well states and found to be considerably smaller than the momentum averaged electron-phonon coupling at the Fermi level of bulk lead, (λ = 1.1-1.7). The results are compared to density functional theory calculations of the lead films with and without interfacial stress. It is shown that the discrepancy can not be explained by means of confinement effects or simple structural modifications of the Pb films and, thus, is attributed to the influence of the substrate on the Pb electronic and vibrational structures. © 2014 IOP Publishing Ltd.

Here the major upgrades of the femtoslicing facility at BESSYII (Khan et al., 2006) are reviewed, giving a tutorial on how elliptical-polarized ultrashort soft X-ray pulses from electron storage rings are generated at high repetition rates. Employing a 6kHz femtosecond-laser system consisting of two amplifiers that are seeded by one Ti:Sa oscillator, the total average flux of photons of 100fs duration (FWHM) has been increased by a factor of 120 to up to 10 6 photons s -1 (0.1% bandwidth) -1 on the sample in the range from 250 to 1400eV. Thanks to a new beamline design, a factor of 20 enhanced flux and improvements of the stability together with the top-up mode of the accelerator have been achieved. The previously unavoidable problem of increased picosecond-background at higher repetition rates, caused by 'halo' photons, has also been solved by hopping between different 'camshaft' bunches in a dedicated fill pattern ('3+1 camshaft fill') of the storage ring. In addition to an increased X-ray performance at variable (linear and elliptical) polarization, the sample excitation in pump-probe experiments has been considerably extended using an optical parametric amplifier that supports the range from the near-UV to the far-IR regime. Dedicated endstations covering ultrafast magnetism experiments based on time-resolved X-ray circular dichroism have been either upgraded or, in the case of time-resolved resonant soft X-ray diffraction and reflection, newly constructed and adapted to femtoslicing requirements. Experiments at low temperatures down to 6K and magnetic fields up to 0.5T are supported. The FemtoSpeX facility is now operated as a 24h user facility enabling a new class of experiments in ultrafast magnetism and in the field of transient phenomena and phase transitions in solids. © 2014 International Union of Crystallography.

A major challenge in understanding the cuprate superconductors is to clarify the nature of the fundamental electronic correlations that lead to the pseudogap phenomenon. Here we use ultrashort light pulses to prepare a non-thermal distribution of excitations and capture novel properties that are hidden at equilibrium. Using a broadband (0.5-2 eV) probe, we are able to track the dynamics of the dielectric function and unveil an anomalous decrease in the scattering rate of the charge carriers in a pseudogap-like region of the temperature (T) and hole-doping (p) phase diagram. In this region, delimited by a well-defined T* neq (p) line, the photoexcitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasiparticles characterized by a longer lifetime. The novel concept of photo-enhanced antinodal conductivity is naturally explained within the single-band Hubbard model, in which the short-range Coulomb repulsion leads to a k-space differentiation between nodal quasiparticles and antinodal excitations. © 2014 Macmillan Publishers Limited. All rights reserved.

The dressing of quasiparticles in solids is investigated by changes in the electronic structure E(k) driven by femtosecond laser pulses. Employing time- and angle-resolved photoemission on an optimally doped cuprate above Tc, we observe two effects with different characteristic temporal evolutions and, therefore, different microscopic origins. First, a marked change in the effective mass due to the 70-meV kink in E(k) is found to occur during the experiment's 100-fs temporal resolution and is assigned to laser-driven perturbation of an electronic interaction dressing the bare band. Second, a change in kF is explained by effective photodoping due to particle-hole asymmetry and offers opportunities for ultrafast optoelectronic switches based on an optically driven insulator-superconductor transition. © 2014 American Physical Society.

After excitation by femtosecond laser pulses, Gd and Tb exhibit ultrafast demagnetization in two steps, with the time constant of the second step linked to the coupling strength of the 4f magnetic moments to the lattice. In time-resolved magneto-optical Kerr effect measurements of Gd1-xTbx alloys, we observe a decrease in this time constant from 33 to 9 ps with Tb content x increasing from 0 to 0.7. We explain this behavior by the stronger spin-lattice coupling of Tb compared to Gd, which increases the effective spin-lattice coupling in Gd1-xTbx with x. In contrast, the faster time constant of the first demagnetization step exhibits no dependence on x. Additional time- and element-resolved x-ray magnetic circular dichroism measurements show a two-step demagnetization of Gd and Tb in Gd0.6Tb0.4 with an equivalent time scale of the second step but a different magnitude of demagnetization which persists for 15 ps. We explain this by an increased coupling of the Gd 4f magnetic moments to the lattice compared to pure Gd, via interatomic exchange coupling to the neighboring Tb 4f moments mediated by 5d electrons, which has limited efficiency and allows an estimation of a characteristic time scale of the interatomic exchange coupling. We assign the first demagnetization step to the dynamics of the laser-excited 5d electrons, while the second demagnetization step is dominated by the strength of spin-lattice coupling of the 4f electrons. © 2014 American Physical Society.

Time- and angle-resolved extreme ultraviolet photoemission spectroscopy is used to study the electronic structure dynamics in BaFe2As2 around the high-symmetry points Γ and M. A global oscillation of the Fermi level at the frequency of the A1g(As) phonon mode is observed. It is argued that this behavior reflects a modulation of the effective chemical potential in the photoexcited surface region that arises from the high sensitivity of the band structure near the Fermi level to the A1g(As) phonon mode combined with a low electron diffusivity perpendicular to the layers. The results establish a novel way to tune the electronic properties of iron pnictides: coherent control of the effective chemical potential. The results further suggest that the equilibration time for the effective chemical potential needs to be considered in the ultrafast electronic structure dynamics of materials with weak interlayer coupling. © 2014 American Physical Society.

The unoccupied electronic structure of epitaxial Pb films on Si(1 1 1) is analyzed by angle-resolved two-photon photoemission in the over(Γ, -) → over(M, -) direction close to the Brillouin zone center. The experimental results are compared to density functional theory calculations and we focus on the nature of the interaction of the 6pz states with the Si substrate. The experimentally obtained dispersion E(k||) of the unoccupied quantum well states is weaker than expected for freestanding films, in good agreement with their occupied counterparts. Following E(k||) of quantum well states as a function of momentum at different energies, which are degenerate and non-degenerate with the Si conduction band, we observe no influence of the Si bulk band and conclude a vanishing direct interaction of the Pb 6pz states with the Si band. However, the momentum range at which mixing of 6pz and 6px,y derived subbands is found to occur in the presence of the Si substrate is closer to over(Γ, -) than in the corresponding freestanding film, which indicates a substrate-mediated enhancement of the mixing of these states. Additional femtosecond time-resolved measurements show a constant relaxation time of hot electrons in unoccupied quantum well states as a function of parallel electron momentum which supports our conclusion of a px,y mediated interaction of the pz states with the Si conduction band. © 2014.

We employed femtosecond time- and angle-resolved photoelectron spectroscopy to analyze the response of the electronic structure of the 122 Fe-pnictide parent compounds Ba/EuFe2As2 and optimally doped BaFe1.85Co0.15As2 near the Γ point to optical excitation by an infrared femtosecond laser pulse. We identify pronounced changes of the electron population within several 100 meV above and below the Fermi level, which we explain as a combination of (i) coherent lattice vibrations, (ii) a hot electron and hole distribution, and (iii) transient modifications of the chemical potential. The responses of the three different materials are very similar. In the coherent response we identify three modes at 5.6, 3.3, and 2.6 THz. While the highest frequency mode is safely assigned to the A1g mode, the other two modes require a discussion in comparison to the literature. Employing a transient three temperature model we deduce from the transient evolution of the electron distribution a rather weak, momentum-averaged electron-phonon coupling quantified by values for λω2 between 30 and 70 meV2. The chemical potential is found to present pronounced transient changes reaching a maximum of 15 meV about 0.6 ps after optical excitation and is modulated by the coherent phonons. This change in the chemical potential is particularly strong in a multiband system like the 122 Fe-pnictide compounds investigated here due to the pronounced variation of the electron density of states close to the equilibrium chemical potential. © 2013 IOP Publishing Ltd.

Vibrational spectroscopy using sum-frequency generation has been used to investigate the coupling between a ferromagnetic thin film and adsorbed molecules, here CO on Ni/Cu(100). The CO stretching vibration exhibits a strong magnetic contrast with a pronounced temperature dependence, underlining the high sensitivity of this adsorbate-specific spectroscopy method. Our results indicate that the strong temperature dependence is caused by dynamical changes in the surface chemical bond when the CO stretch vibration is coupled to thermally excited external vibrational modes. © 2013 AIP Publishing LLC.

Based on the results from femtosecond time-resolved photoemission, we compare three different methods for the determination of the electron-phonon coupling constant λ in Eu- and Ba-based 122 FeAs compounds. We find good agreement between all three methods, which reveal a small λ < 0.2. This makes simple electron-phonon-mediated superconductivity unlikely in these compounds. © IOP Publishing and Deutsche Physikalische Gesellschaft.

We used angle-resolved photoemission spectroscopy (ARPES) and density functional theory calculations to study the electronic structure of Ba(Fe 1-x-yCoxMny)2As2 for x=0.06 and 0 ≥y ≥0.07. From ARPES we derive that the substitution of Fe by Mn does not lead to hole doping, indicating a localization of the induced holes. An evaluation of the measured spectral function does not indicate a diverging effective mass or scattering rate near optimal doping. Thus, the present ARPES results indicate a continuous evolution of the quasiparticle interaction and therefore question previous quantum critical scenarios.

The combination of synchrotron-based soft X-ray light sources and magnetism research has been very fruitful and productive in the last few decades and has led to numerous exciting results. This success is essentially based on resonant dichroic effects, which were employed to analyze magnetic order in an element-specific manner [11, 32]. Thanks to the short wavelength, magneto-dichroic effects could also be employed in microscopy, and within the available momentum transfer even magnetic scattering was developed [11]. Therefore, soft X-ray methods were and still are essential to develop the detailed understanding of magnetism and magnetic materials in the thermodynamic ground state available today. © 2013 Copyright Taylor and Francis Group, LLC.

The femtosecond dynamics of the Fermi surface of DyTe3 and its band structure are investigated by time- and angle-resolved photoemission spectroscopy. We directly monitor the ultrafast collapse of the charge density wave gap within 200 fs. © Owned by the authors, published by EDP Sciences, 2013.

We present time-resolved RHEED from a laser excited Pb(111) surface using a pulse front tilter for the compensation of the velocity mismatch of electrons and light. The laser pulses with tilted fronts were characterized by a spatially resolving cross correlator. The response of the surface upon excitation was observed to be less than 2 ps. © Owned by the authors, published by EDP Sciences, 2013.

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 C 6F 6 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 → π * C 6F 6 LUMO state using time-resolved two-photon photoemission (tr-2PPE) and core-hole-clock (CHC) spectroscopy, respectively. For the molecularly localized core-excited C1s → π * C 6F 6 LUMO state, we separate the intramolecular dynamics from the charge transfer dynamics to the metal substrate by taking the intramolecular dynamics of the free C 6F 6 molecule into account. Our analysis yields a generally applicable description of charge transfer within molecular adsorbates and to the substrate. © 2012 Elsevier B.V. All rights reserved.

This two-volume work covers ultrafast structural and electronic dynamics of elementary processes at solid surfaces and interfaces, presenting the current status of photoinduced processes. Providing valuable introductory information for newcomers to this booming field of research, it investigates concepts and experiments, femtosecond and attosecond time-resolved methods, as well as frequency domain techniques. The whole is rounded off by a look at future developments. © 2012 Wiley-VCH Verlag GmbH & Co. KGaA. All rights reserved.

Here we report on the ultrafast magnetization dynamics of Gd(0001), which we investigated as a function of equilibrium temperature by employing the femtosecond time-resolved magneto-optical Kerr effect (MOKE) and modeling by the Landau-Lifshitz-Bloch equation in combination with the two-temperature model. Based on the observed temperature-dependent transient MOKE signals, we separate the magnetization dynamics into two regimes at delays of (i) a few picoseconds and (ii) several 100 femtoseconds. In the picosecond regime, the demagnetization time determined from the experiment increases with temperature from 0.8 ps at 50 K to 1.5 ps at 280 K. A successful description of this observation was achieved by considering the dynamics of the 4f spin system coupled to 5d conduction electrons within two coupling mechanisms: (a) through electronic scattering and (b) spin-flip scattering mediated by phonons. We conclude that at temperatures below the Debye temperature, a hot electron-mediated process describes the experimentally found demagnetization times of ≈0.8 ps well. At higher temperatures phonon-mediated processes have to be included to explain the 2 times longer demagnetization time. In the second regime at time delays of few 100 fs we find an increase in the MOKE rotation and ellipticity at 50 K at delays before demagnetization sets in. Above 50 K the transient changes in rotation and ellipticity are of opposite sign. We explain this behavior by competing magnetic and nonmagnetic contributions in the transient MOKE signals at these delays directly after optical excitation when excited phonons do not yet facilitate angular momentum transfer to the lattice. © 2012 American Physical Society.

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]. © 2012 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

We investigate the ultrafast electron dynamics of occupied quantum well states (QWSs) in Pb/Si(111) with time-resolved photoemission spectroscopy. We find an ultrafast increase in binding energy of the QWSs driven by the optical excitation, while the electronic system is in a non-equilibrium state. We explain this transient energetic stabilization in the photoexcited state by an ultrafast modification of the Fermi level pinning, triggered by charge transfer across the Pb/Si interface. In addition, we observe the excitation of a coherent surface phonon mode at a frequency of ∼2 THz, which modulates the QWS binding energy. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.

Employing the momentum sensitivity of time- and angle-resolved photoemission spectroscopy we demonstrate the analysis of ultrafast single- and many-particle dynamics in antiferromagnetic EuFe 2As 2. Their separation is based on a temperature-dependent difference of photoexcited hole and electron relaxation times probing the single-particle band and the spin density wave gap, respectively. Reformation of the magnetic order occurs at 800 fs, which is 4 times slower compared to electron-phonon equilibration due to a smaller spin-dependent relaxation phase space. © 2012 American Physical Society.

Understanding strongly correlated rare-earth intermetallic compounds requires knowledge of the nature of the fermionic quasiparticles in states near the Fermi level E F. We report on a pump-probe experiment using femtosecond time- and angle-resolved photoemission spectroscopy to determine lifetimes of hot quasiparticles in the heavy-fermion compound YbRh 2Si 2. An unoccupied band with electronlike dispersion and a band bottom 0.2 eV above E F was identified at Γ̄, in agreement with band structure calculations for the subsurface region. Hot quasiparticle lifetimes from 30 to 80 fs were found for energies between 0.4 and 0.1 eV above E F. These lifetimes generally follow the typical monotonous increase towards E F, in agreement with earlier studies on Yb and Rh elemental metals. However, at normal emission the lifetimes at around 0.2 eV exceed this trend by about +20 fs. This difference decreases with increasing photoemission angle and can be assigned to the particular band that is probed in YbRh 2Si 2. Potential microscopic scenarios are discussed. © 2012 American Physical Society.

Femtosecond x-ray magnetic circular dichroism was used to study the time-dependent magnetic moment of 4f electrons in the ferromagnets Gd and Tb, which are known for their different spin-lattice coupling. We observe a two-step demagnetization with an ultrafast demagnetization time of 750 fs identical for both systems and slower times which differ sizeably with 40 ps for Gd and 8 ps for Tb. We conclude that spin-lattice coupling in the electronically excited state is enhanced up to 50 times compared to equilibrium. © 2011 American Physical Society.

The nonequilibrium state of the high-Tc superconductor Bi 2Sr2CaCu2O8+δ and its ultrafast dynamics have been investigated by femtosecond time- and angle-resolved photoemission spectroscopy well below the critical temperature. We probe optically excited quasiparticles at different electron momenta along the Fermi surface and detect metastable quasiparticles near the antinode, since their decay toward the nodal region through e-e scattering is blocked by phase space restrictions. The observed lack of momentum dependence in the decay rates is in agreement with relaxation dynamics dominated by Cooper pair recombination in a boson bottleneck limit. © 2011 American Physical Society.

The creation and stabilization of localized, low-energy electrons is investigated in polar molecular environments. We create such excess electrons in excited states in ice and ammonia crystallites adsorbed on metal surfaces and observe their relaxation in real time using time-resolved photoelectron spectroscopy. The observed dynamics proceed up to minute timescales and are therefore slowed down considerably compared to ultrafast excited state relaxation in front of metal surfaces, which proceeds typically on femto- or picosecond time scales. It is the highly efficient wave function constriction of the electrons from the metal that ultimately enables the investigation of the relaxation dynamics over a large range of timescales (up to 17 orders of magnitude). Therefore, it gives novel insight into the solvated electron ground state formation at interfaces. As these long-lived electrons are observed for both, D2O and NH3 crystallites, they appear to be of general character for polar molecule-metal interfaces. Their time- and temperature-dependent relaxation is analyzed for both, crystalline ice and ammonia, and compared using an empirical model that yields insight into the fundamental solvation processes of the respective solvent. © The Royal Society of Chemistry 2011.

We have studied the influence of sodium ions bound near the ice/vacuum interface on the electron solvation dynamics in amorphous D2O ice layers by means of femtosecond time-resolved two-photon photoelectron spectroscopy. Adsorption of submonolayer coverages of sodium on top of multilayers of amorphous ice leads to the formation of Na+ ions and to pronounced changes in the observed ultrafast dynamics compared to pure amorphous ice. We identify a Na+-induced species of excess electrons which exhibits a much longer lifetime compared to excess electrons in pure D2O ice and approximate the decay of the Na-induced contribution by two decay times τ2 = 880 fs and τ3 = 9.6 ps. In addition, a faster energetic stabilization of the excited electrons with a rate of σ = 0.73 eV/ps is observed. The population of these electrons depends nonlinearly on the sodium coverage. We attribute the Na-induced contribution to a transient electron/ion/water complex which is located at the ice/vacuum interface. This interpretation is corroborated by coverage-dependent measurements and by overlayer experiments. © 2010 American Chemical Society.

Gaining insights into the mechanisms of how order and broken symmetry emerges from many-particle interactions is a major challenge in solid state physics. Most experimental techniques-such as angle-resolved photoemission spectroscopy (ARPES)-probe the single-particle excitation spectrum and extract information about the ordering mechanism and collective effects, often indirectly through theory. Time-resolved ARPES (tr-ARPES) makes collective dynamics of a system after optical excitation directly visible through their influence on the quasi-particle band structure. Using this technique, we present a systematic study of TbTe3, a metal that exhibits a charge-density wave (CDW) transition. We discuss time-resolved data taken at different positions in the Brillouin zone (BZ) and at different temperatures. © IOP Publishing Ltd and Deutsche Physikalische Gesellschaft.

Ultrafast laser-induced demagnetization of Gd(0001) has been investigated by magneto-induced optical second harmonic generation and the magneto-optical Kerr effect which facilitate a comparison of surface and bulk dynamics. We observe pronounced differences in the transient changes of the surface and bulk sensitive magneto-optical signals which we attribute to transfer of optically excited, spin-polarized carriers between surface and bulk states of the Gd(0001) film. A fluence dependent analysis of the bulk magnetization dynamics results in a weak variation of the demagnetization time constant, which starts at about 0.7ps and increases by 10% within a fluence variation up to 1mJ/cm2. We compare these results with fluence dependent changes in the transient energy density calculated by the two temperature model. The determined characteristic times of excess energy transfer from the electron system to the lattice, which is mediated by e-ph scattering, range from 0.2 to 0.6ps. Such a more pronounced fluence dependent change in the characteristic time compared to the observed rather weakly varying demagnetization times suggests a more advanced description of the optically excited state than by the two-temperature model. © 2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Hot carrier-induced spin dynamics is analyzed in epitaxial Au/Fe/MgO(001) by a time domain approach. We excite a spin current pulse in Fe by 35 fs laser pulses. The transient spin polarization, which is probed at the Au surface by optical second harmonic generation, changes its sign after a few hundred femtoseconds. This is explained by a competition of ballistic and diffusive propagation considering energy-dependent hot carrier relaxation rates. In addition, we observe the decay of the spin polarization within 1 ps, which is associated with the hot carrier spin relaxation time in Au. © 2011 American Physical Society.

Quasiparticle lifetimes in metals as described by Fermi-liquid theory are essential in surface chemistry and determine the mean free path of hot carriers. Relaxation of hot electrons is governed by inelastic electron-electron scattering, which occurs on femtosecond timescales owing to the large scattering phase space competing with screening effects. Such lifetimes are widely studied by time-resolved two-photon photoemission, which led to understanding of electronic decay at surfaces. In contrast, quasiparticle lifetimes of metal bulk and films are not well understood because electronic transport leads to experimental lifetimes shorter than expected theoretically. Here, we lift this discrepancy by investigating Pb quantum-well structures on Si(111), a two-dimensional model system. For electronic states confined to the film by the Si bandgap we find quantitative agreement with Fermi-liquid theory and ab initio calculations for bulk Pb, which we attribute to efficient screening. For states resonant with Si bands, extra decay channels open for electron transfer to Si, resulting in lifetimes shorter than expected for bulk. Thereby we demonstrate that for understanding electronic decay in nanostructures coupling to the environment is essential, and that even for electron confinement to a few ångströms Fermi-liquid theory for bulk can remain valid. © 2010 Macmillan Publishers Limited. All rights reserved.

The polarization of the two beam (driver-probe) high-order harmonic generation from solids is measured. The experiments, together with computer simulations, allow us to distinguish two different coupling mechanisms of the driver and the probe, resulting in different harmonic efficiencies and spectral slopes. We find that in the nonrelativistic regime the coupling is mostly due to the nonlinear plasma density modulation. © 2010 The American Physical Society.