Search

The semiconductor ReSe$_2$ is characterized by a strongly anisotropic optical absorption and is therefore promising as an optically active component in two-dimensional heterostructures. However, the underlying femtosecond dynamics of photoinduced excitations in such materials has not been sufficiently explored. Here, we apply an infrared optical excitation to single-layer ReSe$_2$ grown on a bilayer graphene substrate and monitor the temporal evolution of the excited state signal using time- and angle-resolved photoemission spectroscopy. We measure an optical gap of $(1.53 \pm 0.02)$ eV, consistent with resonant excitation of the lowest exciton state. The exciton distribution is tunable via the linear polarization of the pump pulse and exhibits a biexponential decay with time constants given by $\tau_1 = (110 \pm 10)$ fs and $\tau_2 = (650 \pm 70)$ fs, facilitated by recombination via an in-gap state that is pinned at the Fermi level. By extracting the momentum-resolved exciton distribution we estimate its real-space radial extent to be greater than 17.1 \AA, implying significant exciton delocalization due to screening from the bilayer graphene substrate., Comment: 6 pages, 4 figures

The presence of the term $\left(\case{v}{c}\right)$ that characterizes the electrodynamic retarded potentials, also known as Li\'enard-Wiechert potentials, is thought to be reminiscent of a Doppler effect. Here, we show that these potentials are consistent with the Doppler shifted electromagnetic (e.m.) field generated by a charge moving along a generic trajectory with respect to the laboratory reference frame. Of course, the retarded potentials derived here are formally the same as those reported in the current literature. Nonetheless, this work sheds a new light on the origin of the electrodynamics retarded fields, while offering a direct physical interpretation of the term $\left(\case{v}{c}\right)$ characterizing the related potentials., Comment: 11 pages, 1 figure

Understanding how a spin current flows across metal-semiconductor interfaces at pico- and femtosecond time scales is of paramount importance for ultrafast spintronics, data processing, and storage applications. However, the possibility to directly access the propagation of spin currents, within such time scales, has been hampered by the simultaneous lack of both ultrafast element-specific magnetic sensitive probes and tailored well-built and characterized metal-semiconductor interfaces. Here, by means of a novel free-electron laser-based element-sensitive ultrafast time-resolved Kerr spectroscopy, we reveal different magnetodynamics for the Ni M 2 , 3 and Si L 2 , 3 absorption edges. These results are assumed to be the experimental evidence of photoinduced spin currents propagating at a speed of ∼ 0.2 nm/fs across the Ni/Si interface.

FeSe x Te 1 − x compounds display a rich phase diagram, ranging from the nematicity of FeSe to the ( π , π ) magnetism of FeTe. We focus on FeSe0.4Te0.6, and exploit tr-ARPES to study its ultrafast electron dynamics following photoexcitation by near-infrared pump pulses. By exploiting probe-polarization-dependent matrix element effects, we reveal a photoinduced long-lived state, lasting for a few tens of picoseconds, showing features compatible with a nematic state. The possibility to induce a long-lived state in this compound by using ultra-short pulses might shed a new light on the driving force behind the nematic symmetry breaking in iron-based superconductors. With the aid of a phenomenological model, we illustrate how our results possibly question the common belief that a low-energy coupling with fluctuations is a necessary condition to stabilize the nematic order. On the contrary, the tendency towards orbital differentiation due to strong electronic correlations induced by the Hund’s coupling could be at the origin of the nematic order in iron-based superconductors.

Here, we report on the conceptual design, the hardware realization, and the first experimental results of a novel and compact x-ray polarimeter capable of a single-pulse linear polarization angle detection in the extreme ultraviolet photon energy range. The polarimeter is tested by performing time resolved pump-probe experiments on a Ni80Fe20 Permalloy film at the M-2,M-3 Ni edge at an externally seeded free-electron laser source. Comparison with similar experiments reported in the literature shows the advantages of our approach also in view of future experiments.

Time-resolved optical spectroscopy (TR-OS) has emerged as a fundamental spectroscopic tool for probing complex materials, to both investigate ground-state-related properties and trigger phase transitions among different states with peculiar electronic and lattice structures. We describe a versatile approach to perform polarization-resolved TR-OS measurements, by combining broadband detection with the capability to simultaneously probe two orthogonal polarization states. This method allows us to probe, with femtoseconds resolution, the frequency-resolved reflectivity or transmittivity variations along two mutually orthogonal directions, matching the principal axis of the crystal structure of the material under scrutiny. We report on the results obtained by acquiring the polarization-dependent transient reflectivity of two polytypes of the MoTe2 compound, with 2H and 1T’ crystal structures. We reveal marked anisotropies in the time-resolved reflectivity signal of 1T’-MoTe2, which are connected to the crystal structure of the compound. Polarization- and time- resolved spectroscopic measurements can thus provide information about the nature and dynamics of both the electronic and crystal lattice subsystems, advancing the comprehension of their inter-dependence, in particular in the case of photoinduced phase transitions; in addition, they provide a broadband measurement of transient polarization rotations.

The quest for mapping the femtosecond dynamics of the electronic band structure of complex materials over their full first Brillouin zone is pushing the development of schemes to efficiently generate ultrashort photon pulses in the VUV energy range. At present, the critical aspect in time- and angle-resolved photoelectron spectroscopy (TR-ARPES) is to combine a high photon energy with high photoemission count rates and a narrow pulse-bandwidth, necessary to achieve high energy resolution, while preserving a good time resolution and mitigating space-charge effects. Here we describe a novel approach to produce light pulses at 10.8 eV, combining high repetition rate operation (1–4 MHz), high energy resolution ( ∼ 26 meV) and space-charge free operation, with a time-resolution of ∼ 700 fs. These results have been achieved by generating the ninth harmonic of a Yb fiber laser, through a phase-matched process of third harmonic generation in Xenon of the laser third harmonic. The full up-conversion process is driven by a seed pulse energy as low as 10 μ J, hence is easily scalable to multi-MHz operation. This source opens the way to TR-ARPES experiments for the investigation of the electron dynamics over the full first Brillouin zone of most complex materials, with unprecedented energy and momentum resolutions and high count rates. The performances of the setup are tested by TR-ARPES on the topological insulator Bi 2 Se 3 .

Here we show how time-resolved broadband optical spectroscopy can be used to quantify, with femtometer resolution, the oscillation amplitudes of coherent phonons through a displacive model without free tuning parameters, except an overall scaling factor determined by comparison between experimental data and density functional theory calculations. $WTe_2$ is used to benchmark this approach. In this semimetal, the response is anisotropic and provides the spectral fingerprints of two $A_1$ optical phonons at $\sim$8 and $\sim$80 $cm^-$$^1$. In principle, this methodology can be extended to any material in which an ultrafast excitation triggers coherent lattice modes modulating the high-energy optical properties., Comment: Main Text 5 pages 4 figures, Supplemental Material 20 pages 18 figures

A novel ultrafast photoemission technique unveils the Mottness of antinodal quasiparticles in superconducting copper oxides., Many puzzling properties of high–critical temperature (Tc) superconducting (HTSC) copper oxides have deep roots in the nature of the antinodal quasiparticles, the elementary excitations with wave vector parallel to the Cu–O bonds. These electronic states are most affected by the onset of antiferromagnetic correlations and charge instabilities, and they host the maximum of the anisotropic superconducting gap and pseudogap. We use time-resolved extreme-ultraviolet photoemission with proper photon energy (18 eV) and time resolution (50 fs) to disclose the ultrafast dynamics of the antinodal states in a prototypical HTSC cuprate. After photoinducing a nonthermal charge redistribution within the Cu and O orbitals, we reveal a dramatic momentum-space differentiation of the transient electron dynamics. Whereas the nodal quasiparticle distribution is heated up as in a conventional metal, new quasiparticle states transiently emerge at the antinodes, similarly to what is expected for a photoexcited Mott insulator, where the frozen charges can be released by an impulsive excitation. This transient antinodal metallicity is mapped into the dynamics of the O-2p bands, thus directly demonstrating the intertwining between the low- and high-energy scales that is typical of correlated materials. Our results suggest that the correlation-driven freezing of the electrons moving along the Cu–O bonds, analogous to the Mott localization mechanism, constitutes the starting point for any model of high-Tc superconductivity and other exotic phases of HTSC cuprates.

Femtosecond laser excitations in half-metal (HM) compounds are theoretically predicted to induce an exotic picosecond spin dynamics. In particular, conversely to what is observed in conventional metals and semiconductors, the thermalization process in HMs leads to a long living partially thermalized configuration characterized by three Fermi-Dirac distributions for the minority, majority conduction, and majority valence electrons, respectively. Remarkably, these distributions have the same temperature but different chemical potentials. This unusual thermodynamic state is causing a persistent nonequilibrium spin polarization only well above the Fermi energy. Femtosecond spin dynamics experiments performed on Fe3O4 by time- and spin-resolved photoelectron spectroscopy support our model. Furthermore, the spin polarization response proves to be very robust and it can be adopted to selectively test the bulk HM character in a wide range of compounds. Funding Agencies|UK EPSRC Grant [GR/M50447]; STFC; FERMI FEL project; Austrian Science Fund (FWF) through Lise Meitner Grant [M1925-N28]; Nanyang Technological University, NAP-SUG; CEDAMNF [CZ 02.1.01/0.0/0.0/15_003/0000358]; ERDF

Multiorbital correlated materials are often on the verge of multiple electronic phases (metallic, insulating, superconducting, charge and orbitally ordered), which can be explored and controlled by small changes of the external parameters. The use of ultrashort light pulses as a mean to transiently modify the band population is leading to fundamentally new results. In this paper we will review recent advances in the field and we will discuss the possibility of manipulating the orbital polarization in correlated multi-band solid state systems. This technique can provide new understanding of the ground state properties of many interesting classes of quantum materials and offers a new tool to induce transient emergent properties with no counterpart at equilibrium. We will address: the discovery of high-energy Mottness in superconducting copper oxides and its impact on our understanding of the cuprate phase diagram; the instability of the Mott insulating phase in photoexcited vanadium oxides; the manipulation of orbital-selective correlations in iron-based superconductors; the pumping of local electronic excitons and the consequent transient effective quasiparticle cooling in alkali-doped fullerides. Finally, we will discuss a novel route to manipulate the orbital polarization in a a k-resolved fashion. © 2018 COPYRIGHT SPIE. Downloading of the abstract is permitted for personal use only.

Here we report on experiments performed by linear-dichroism angle resolved photoelectron spectroscopy (LD-ARPES) on septuple layers (SL) topological insulator GeBi2Te4. The linear dichroic signals, both for the valence band states and in the topologically protected surface state are interpreted as a probe of the symmetry of the states. The observation of a change in the LD-ARPES spectrum at the top of VB is attributed to the band parity inversion which is predicted by theory for all materials entering the topologically protected phase. Finally, the opening of a gap in the surface state dispersion along the non-high symmetry direction is reported. This is proposed to originated from the interaction between the surface state and the VB, leading to the formation of surface resonances.

The prediction of Weyl fermions in the low-temperature noncentrosymmetric $1{T}^{\ensuremath{'}}$ phase of ${\mathrm{MoTe}}_{2}$ still awaits clear experimental confirmation. Here, we report angle-resolved photoemission (ARPES) data and ab initio calculations that reveal a surface state arc dispersing between the valence and the conduction band, as expected for a Weyl semimetal. However, we find that the arc survives in the high-temperature centrosymmetric $1{T}^{\ensuremath{'}\ensuremath{'}}$ phase. Therefore, a surface Fermi arc is not an unambiguous fingerprint of a topologically nontrivial phase. We have also investigated the surface state spin texture of the $1{T}^{\ensuremath{'}}$ phase by spin-resolved ARPES, and identified additional topologically trivial spin-split states within the projected band gap at higher binding energies.

Physical review / B 96(24), 241408 (2017). doi:10.1103/PhysRevB.96.241408, $MoTe_2$ has recently been shown to realize in its low-temperature phase the type-II Weyl semimetal (WSM). We investigated by time- and angle- resolved photoelectron spectroscopy (tr-ARPES) the possible influence of the Weyl points on the electron dynamics above the Fermi level $E_F$, by comparing the ultrafast response of $MoTe_2$in the trivial and topological phases. In the low-temperature WSM phase, we report an enhanced relaxation rate of electrons optically excited to the conduction band, which we interpret as a fingerprint of the local gap closure when Weyl points form. By contrast, we find that the electron dynamics of the related compound $WTe_2$is slower and temperature independent, consistent with a topologically trivial nature of this material. Our results shows that tr-ARPES is sensitive to the small modifications of the unoccupied band structure accompanying the structural and topological phase transition of $MoTe_2$., Published by Inst., Woodbury, NY

The electronic structure of ZrTe5 has been matter of renewed interest aimed at clarifying, along with its topological character, the temperature dependence of the unusual transport properties of this material. Here, we report an extensive high resolution Angle Resolved Photoelectron Spectroscopy (ARPES) study unveiling a non-monotonic shift of the bands, when the sample temperature is varied between 16 K and 300 K. Moreover, the present conventional ARPES and circularly dichroic ARPES measurements reveal the presence of two states at the top of the valence band. The strong ARPES dichroic signal detected in proximity of the Fermi energy has been interpreted as the indication of the presence of spin polarized states, in agreement with the predicted strong topological character of this material. published

Physical review / B 96(18), 184420 (2017). doi:10.1103/PhysRevB.96.184420, We report a high-resolution resonant inelastic extreme ultraviolet (EUV) scattering study of the quantum Heisenberg antiferromagnet KCoF$_3$. By tuning the EUV photon energy to the cobalt M$_{23}$ edge, a complete set of low-energy 3d spin-orbital excitations is revealed. These low-lying electronic excitations are modeled using an extended multiplet-based mean-field calculation to identify the roles of lattice and magnetic degrees of freedom in modifying the resonant inelastic x-ray scattering (RIXS) spectral line shape. We have demonstrated that the temperature dependence of RIXS features upon the antiferromagnetic ordering transition enables us to probe the energetics of short-range spin correlations in this material., Published by APS, Woodbury, NY

We study the photoinduced insulator-metal transition in V O2, correlating its threshold and dynamics with excitation wavelength. In single crystals, switching can only be induced with photon energies above the 670 meV gap. This contrasts with the case of polycrystalline films, where formation of the metallic state can be initiated also with photon energies as low as 180 meV, which are well below the bandgap. Perfection of this process may become conducive to schemes for optical switches, limiters, and detectors operating at room temperature in the mid-infrared. © 2008 American Institute of Physics.

The non-equilibrium approach to correlated electron systems is often based on the paradigm that different degrees of freedom interact on different timescales. In this context, photo-excitation is treated as an impulsive injection of electronic energy that is transferred to other degrees of freedom only at later times. Here, by studying the ultrafast dynamics of quasi-particles in an archetypal strongly correlated charge-transfer insulator (La2CuO4+delta), we show that the interaction between electrons and bosons manifests itself directly in the photo-excitation processes of a correlated material. With the aid of a general theoretical framework (Hubbard-Holstein Hamiltonian), we reveal that sub-gap excitation pilots the formation of itinerant quasi-particles, which are suddenly dressed by an ultrafast reaction of the bosonic field.

The complex electronic properties of ${\mathrm{ZrTe}}_{5}$ have recently stimulated in-depth investigations that assigned this material to either a topological insulator or a 3D Dirac semimetal phase. Here we report a comprehensive experimental and theoretical study of both electronic and structural properties of ${\mathrm{ZrTe}}_{5}$, revealing that the bulk material is a strong topological insulator (STI). By means of angle-resolved photoelectron spectroscopy, we identify at the top of the valence band both a surface and a bulk state. The dispersion of these bands is well captured by ab initio calculations for the STI case, for the specific interlayer distance measured in our x-ray diffraction study. Furthermore, these findings are supported by scanning tunneling spectroscopy revealing the metallic character of the sample surface, thus confirming the strong topological nature of ${\mathrm{ZrTe}}_{5}$.

Solid Si under intense femtosecond irradiation is investigated over a wide range of fluences below the melting transition by supercontinuum light (400--800 nm) transient reflectivity. By solving a system of time-dependent equations, the fast and slow components of the energy and carriers diffusion can be disentangled from the reflectivity data, providing considerable insight into the nonequilibrium phase-change dynamics. The study of the fluence values immediately preceding the dramatic melting transition can be useful for discriminating between the thermal and electronic origins of the disordering of the structure by looking at the modification of the solid-state properties of the Si surface.

We present equilibrium and out-of-equilibrium studies of the Verwey transition in magnetite. In the equilibrium optical conductivity, we find a steplike change at the phase transition for photon energies below about 2 eV. The possibility of triggering a nonequilibrium transient metallic state in insulating magnetite by photo excitation was recently demonstrated by an x-ray study. Here we report a full characterization of the optical properties in the visible frequency range across the nonequilibrium phase transition. Our analysis of the spectral features is based on a detailed description of the equilibrium properties. The out-of-equilibrium optical data bear the initial electronic response associated to localized photoexcitation, the occurrence of phase separation, and the transition to a transient metallic phase for excitation density larger than a critical value. This allows us to identify the electronic nature of the transient state, to unveil the phase transition dynamics, and to study the consequences of phase separation on the reflectivity, suggesting a spectroscopic feature that may be generally linked to out-of-equilibrium phase separation.

International audience; SmB6 is a mixed valence Kondo system resulting from the hybridization between localized f electrons and delocalized d electrons. We have investigated its out-of-equilibrium electron dynamics by means of time- and angle-resolved photoelectron spectroscopy. The transient electronic population above the Fermi level can be described by a time-dependent Fermi-Dirac distribution. By solving a two-temperature model that well reproduces the relaxation dynamics of the effective electronic temperature, we estimate the electron-phonon coupling constant lambda to range from 0.13 +/- 0.03 to 0.04 +/- 0.01. These extremes are obtained assuming a coupling of the electrons with either a phonon mode at 10 or 19 meV. A realistic value of the average phonon energy will give an actual value of lambda within this range. Our results provide an experimental report on the material electron-phonon coupling, contributing to both the electronic transport and the macroscopic thermodynamic properties of SmB6.

Many-body interactions with the underlying bulk electrons determine the properties of confined electronic states at the surface of a metal. Using momentum resolved nonlinear photoelectron spectroscopy we show that one can tailor these many-body interactions in graphite, leading to a strong renormalization of the dispersion and linewidth of the image potential state. These observations are interpreted in terms of a basic self-energy model, and may be considered as exemplary for optically induced many-body interactions.

By tuning the laser photon energy in the non-linear two-photons photoemission at a single-layer graphene/Cu(111) interface, it is possible to observe a strong resonance at h upsilon = 3.5 eV along with a weaker one at h upsilon = 3.85 eV. The main resonance photon energy is consistent with a direct optical transition between the occupied Cu(111) Shockley surface state and the n = 1 image potential state, located in the real gap-space between the single-layer graphene and the Cu( Ill) surface. The large amplitude of this resonance unveils a high value of the electric dipole matrix element integral that governs this transition. Furthermore, the Lorentzian shape of this resonance implies that these two states are decoupled from the continuum of states and the lifetime of the image potential state can be estimated. (C) 2015 Elsevier B.V. All rights reserved.

The quest for investigating the non-equilibrium dynamics of the band structure of strongly-correlated materials over their entire Brillouin zone is a primary objective. However, the actual ultrafast UV light sources are not suitable for addressing several critical questions in the field. Here we report on a novel light source generating sub-250 fs, 9.3 eV photon energy light pulses at 250 kHz repetition rate, obtained via third-harmonic generation in Xe of frequency-doubled 50 fs laser pulses at 1.55 eV. By reporting the measured band dispersion of a Cu(111) crystal and the non-equilibrium dynamics of the Bi2Se3 topological insulator, we prove that this source is suitable for studying the non-equilibrium dynamics of the entire Fermi surface of several complex materials, with high signal statistics and limited space-charge effect. (C) 2015 Elsevier B.V. All rights reserved.

Using time-resolved reflectivity measurements on unaligned and aligned bundled single-wall carbon nanotubes with a pump energy of 1.55 eV, quasi-resonant with the second Van Hoye singularity of semiconducting tubes, a positive sign of the transient reflectivity is detected in unaligned nanotubes. In contrast a negative sign is detected in aligned nanotubes. This discovery addresses a long-standing question showing that in unaligned nanotubes the stronger intertube interactions favor the formation of short-lived free charge carriers in semiconducting tubes. A detailed analysis of the transient reflectivity spectral response shows that the free carriers in the photo-excited state of semiconducting tubes move towards metallic tubes in about 400 fs. (C) 2011 Elsevier Ltd. All rights reserved.

Optical homodyne tomography consists in reconstructing the quantum state of an optical field from repeated measurements of its amplitude at different field phases (homodyne data). The experimental noise, which unavoidably affects the homodyne data, leads to a detection efficiency $\eta 0.5$ ) below which quantum features, like quantum interferences, cannot be retrieved. Here, by numerical experiments, we demonstrate that quantum interferences can be effectively reconstructed also for low homodyne detection efficiency. In particular, we address the challenging case of a Schrodinger cat state and test the minimax and adaptive Wigner function reconstruction technique by processing homodyne data distributed according to the chosen state but with an efficiency $\eta< 0.5$ . By numerically reproducing the Schrodinger’s cat interference pattern, we give evidence that quantum state reconstruction is actually possible in these conditions, and provide a guideline for handling optical tomography based on homodyne data collected by low efficiency detectors.

Single-layer graphene supported on a metal surface has shown remarkable properties relevant for novel electronic and optoelectronic devices. However, the nature of the electronic states derived from unoccupied surface states and quantum well states, lying in the real-space gap between the graphene and the solid surface, has not been explored and exploited yet. Herein, we use ultraviolet nonlinear angle-resolved photoemission spectroscopy to unveil the coexistence at the graphene/Cu(111) interface of a highest occupied Shockley surface state (HOSS) and the two lowest unoccupied surface states (LUSS). The experimental results and electronic structure calculations, based on one-dimensional model potential, indicate that the two unoccupied states originate from the hybridization of an n = 1 image potential state with a quantum well state. The hybridized nature of these unoccupied states is benchmarked by a similar experiment done on single-layer graphene grown on copper polycrystalline foil where only the image state survives being the quantum well state at this interface inhibited.

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation., 17 pages, 3 figures

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, unveiling an anomalous decrease of 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 photo-excitation process triggers the evolution of antinodal excitations from gapped (localized) to delocalized quasi-particles 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., accepted for publication on Nature Communications

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tuneable band gap. However, no consistent picture of the gap's effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second sub-state of the conduction band, in which the excited electrons decay through fast, phonon-assisted inter-band transitions., Comment: 5 pages, 4 figures

Pulsed homodyne quantum tomography usually requires a high detection efficiency limiting its applicability in quantum optics. Here, it is shown that the presence of low detection efficiency ($

Nature materials 12(10), 882 - 886 (2013). doi:10.1038/nmat3718, As the oldest known magnetic material, magnetite (Fe3O4) has fascinated mankind for millennia. As the first oxide in which a relationship between electrical conductivity and fluctuating/localized electronic order was shown1, magnetite represents a model system for understanding correlated oxides in general. Nevertheless, the exact mechanism of the insulator–metal, or Verwey, transition has long remained inaccessible. Recently, three-Fe-site lattice distortions called trimerons were identified as the characteristic building blocks of the low-temperature insulating electronically ordered phase9. Here we investigate the Verwey transition with pump–probe X-ray diffraction and optical reflectivity techniques, and show how trimerons become mobile across the insulator–metal transition. We find this to be a two-step process. After an initial 300 fs destruction of individual trimerons, phase separation occurs on a 1.5±0.2 ps timescale to yield residual insulating and metallic regions. This work establishes the speed limit for switching in future oxide electronics, Published by Nature Publishing Group, Basingstoke

In strongly correlated materials the electronic and optical properties are significantly affected by the coupling of fermionic quasiparticles to different degrees of freedom, such as lattice vibrations and bosonic excitations of electronic origin. Broadband ultrafast spectroscopy is emerging as the premier technique to unravel the subtle interplay between quasiparticles and electronic or phononic collective excitations, by their different characteristic timescales and spectral responses. By investigating the femtosecond dynamics of the optical properties of Y-Bi2212 crystals over the 0.5-2 eV energy range, we disentangle the electronic and phononic contributions to the generalized electron-boson Eliashberg function, showing that the spectral distribution of the electronic excitations, such as spin fluctuations and current loops, and the strength of their interaction with quasiparticles can account for the high critical temperature of the superconducting phase transition. Finally, we discuss how the use of this technique can be extended to the underdoped region of the phase diagram of cuprates, in which a pseudogap in the quasiparticle density of states opens. The microscopic modeling of the interaction of ultrashort light pulses with unconventional superconductors will be one of the key challenges of the next-years materials science, eventually leading to the full understanding of the role of the electronic correlations in controlling the dynamics on the femtosecond timescale., Comment: 15 pages, 5 figures, Invited manuscript for the proceedings of "Materials & Mechanisms of Superconductivity" (M2S), Washington, 2012

The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and playsa central role for many electronic and optoelectronic applications. Harvesting energy from excitedelectron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energyto vibrations, merely heating the lattice. Until now, the hot carrier dynamics in graphene could only beaccessed indirectly. Here, we present a dynamical view on the Dirac cone by time- and angle-resolvedphotoemission spectroscopy. This allows us to show the quasi-instant thermalization of the electron gas toa temperature of 2000 K, to determine the time-resolved carrier density, and to disentangle the subsequentdecay into excitations of optical phonons and acoustic phonons (directly and via supercollisions).

We report the first generation of coherent, tunable, variable-polarization, soft X-ray femtosecond pulses, generated by a seeded free-electron laser (FEL) operating in the fresh bunch, two-stage harmonic upshift configuration. Characterization of the radiation proves this FEL configuration can produce single-transverse-mode, narrow-spectral-bandwidth output pulses of several tens of microjoules energy and low pulse-to-pulse wavelength jitter at final wavelengths of 10.8 nm and below. The fresh bunch configuration enhances the FEL emission at high harmonic orders by avoiding a gain depression due to the energy spread induced by the first-stage FEL interaction. Coherent signals measured down to 4.3 nm suggest this configuration is directly scalable to photon energies that will enable scientific investigations below the carbon K-edge, including access to the L-edges of many magnetic materials, with an energy per pulse unlocking the gate for experiments in the soft X-ray region with close to Fourier-transform-limited pulses. © 2013 Macmillan Publishers Limited. All rights reserved.