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International audience; Replying to D. Moreno-Mencía et al. Nature Communicationshttps://doi.org/10.1038/s41467-019-11743-3 (2019).

International audience; We describe some general features in the transient behaviour of strongly correlated transition metal oxides, following ultrafast excitation by a femtosecond laser pulse. Our analysis is based on time-resolved reflectivity measurements on (V1-xCrx)2O3, a prototype Mott-Hubbard material, and the manganite compound (La0.67Sr0.33)MnO3, performed over a time window of several tenths of ps. We point out the contribution of coherent lattice oscillations-both optical and acoustic-to the overall signal, and show how they can depend on the crystallographic orientation of the material with respect to the laser beam wavevector and polarisation. In particular, an acoustic wave is always found to be present in our measurements, and we show that its oscillating behaviour is superposed to the average time evolution of the material, which can be instead related in different ways to its electronic properties and thermodynamic phase. All these effects are to be taken into account in any further analysis leading to the estimation of relevant physical parameters for correlated materials, and they appear to play a significant role not only for reflectivity techniques, but also in other kinds of ultrafast pump-probe experiments.

Imaging of flux vortices in high quality MgB$_2$ single crystals has been successfully performed in a commercial Field Emission Gun-based Transmission Electron Microscope. In Cryo-Lorentz Microscopy, the sample quality and the vortex lattice can be monitored simultaneously, allowing one to relate microscopically the surface quality and the vortex dynamics. Such a vortex motion ultimately determines the flow resistivity, $\rho_{f}$, the knowledge of which is indispensable for practical applications such as superconducting magnets or wires for Magnetic Resonance Imaging. The observed patterns have been analyzed and compared with other studies by Cryo-Lorentz Microscopy or Bitter decoration. We find that the vortex lattice arrangement depends strongly on the surface quality obtained during the specimen preparation, and tends to form an hexagonal Abrikosov lattice at a relatively low magnetic field. Stripes or gossamer-like patterns, recently suggested as potential signatures of an unconventional behavior of MgB$_2$, were not observed.

Ultrafast Electron Diffraction (UED) has been widely used to investigate the structural dynamics of molecules and materials. Femtosecond (fs) electron bunches are used to obtain diffraction images of a specimen upon photo-excitation by a temporally delayed light pulse. The high cross-section of electrons makes it a very flexible tool for the study of light elements, monolayers and surfaces; at the same time, electrons can travel down to few nanometers (nm) and structural information from the bulk can also be retrieved. In this article, we discuss the design and implementation of a flexible beamline for fs electron diffraction experiments in transmission or reflection geometry. By the use of a radiofrequency (RF) compression cavity synchronized to our laser system, in combination with a set of electron optics, we demonstrate that we can control the beam properties in terms of charge per pulse, transverse spot-size on the sample and temporal duration of the bunches. The characterization of the beam is performed via a light-electrons cross-correlation experiment and we demonstrate an overall temporal resolution around 300 fs for bunches containing up to 10(5) electrons at a repetition rate of 20 kHz. (c) 2012 Elsevier B.V. All rights reserved.

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their reequilibration by monitoring the transient lattice temperature through femtosecond x-ray diffraction in La2-xSrxCuO4 single crystals with x = 0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the ab initio calculated shape of the electronic density of states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular, in superconductors.

The strength of the electron-phonon coupling parameter and its evolution throughout a solid's phase diagram often determines phenomena such as superconductivity, charge- and spin-density waves. Its experimental determination relies on the ability to distinguish thermally activated phonons from those emitted by conduction band electrons, which can be achieved in an elegant way by ultrafast techniques. Separating the electronic from the out-of-equilibrium lattice subsystems, we probed their reequilibration by monitoring the transient lattice temperature through femtosecond x-ray diffraction in La2−xSrxCuO4 single crystals with x = 0.1 and 0.21. The temperature dependence of the electron-phonon coupling is obtained experimentally and shows similar trends to what is expected from the ab initio calculated shape of the electronic density of states near the Fermi energy. This study evidences the important role of band effects in the electron-lattice interaction in solids, in particular, in superconductors.

We present an angle-resolved photoelectron spectroscopy study of the changes in the electronic structure of electron-doped Ba(Fe1-xCox)(2)As-2 across the superconducting phase transition. By changing the polarization of the incoming light, we were able to observe the opening of the gap for the inner hole pocket alpha and to compare its behavior with the outer holelike band beta. Measurements along high-symmetry directions show that the behavior of beta is consistent with an isotropic gap opening, while slight anisotropies are detected for the inner band alpha. The implications of these results for the s +/- symmetry of the superconducting order parameter are discussed, in relation to the nature of the different iron orbitals contributing to the electronic structure of this multiband system.

Nature Communications 1, Article number: 105 (2010); published: 02 November 2010; updated: 17 January 2012. In Figure 2 of this Article, panel labels c and d were inadvertently switched. A typographical error was also introduced in the last sentence of the legend, which should have read 'The scale bar in panel c represents 10 μm'.

We present a spectromicroscopy study of the two distinct metal-insulator transitions in (V1-xCrx)(2)O-3, x = 0.011. The coexistence of metallic and insulating domains was observed with scanning photoelectron microscopy for both the paramagnetic insulator-paramagnetic metal and paramagnetic metal-antiferromagnetic insulator transitions, evidencing a clear correlation between their nucleation regions. Although these two transitions are very different in nature and underlying mechanism, in both cases the morphology of their phase separation is influenced by structural inhomogeneities. These results demonstrate the general relevance of strain caused by local lattice distortions in guiding the intrinsic tendency towards phase separation in Mott materials. (C) 2012 American Institute of Physics. [doi: 10.1063/1.3675445]

We report a high-momentum and energy resolution angle-resolved photoemission study of superconducting Ba(Fe${}_{1\ensuremath{-}x}$Co${}_{x}$)${}_{2}$As${}_{2}$. Polarization-dependent measurements performed at low photon energy along high-symmetry directions in the Brillouin zone made it possible to get new insight into the role of the five Fe 3$d$ orbitals in the complex electronic structure of this compound close to the Fermi level, in particular, into the nature of the holelike pockets. Two distinct inner $\ensuremath{\alpha}$ pockets could be disentangled, suggesting that their origin is probably due to hybridized ${d}_{\mathit{xz}}$ and ${d}_{\mathit{yz}}$. We also show that the complex outer $\ensuremath{\beta}$ pocket is mainly of ${d}_{{z}^{2}}$ nature, with contributions of other orbitals of different symmetry only in specific points of the Brillouin zone, in the proximity of the ${k}_{z}=$1 $[4\ensuremath{\pi}/c]$ plane. The identification of a ${d}_{{z}^{2}}$ nature for $\ensuremath{\beta}$ contributes to our understanding of the role of electron correlations in 122 pnictide superconductors and of the enhancement of the three-dimensional character of the Fermi surface in Co-doped compounds.

The transient reflectivity response of phase-change Ge2 Sb 2 Te5 films to intense femtosecond laser pulses is studied by ultrafast coherent phonon spectroscopy. The three different phases (amorphous, fcc-, and hcp-crystalline), as well as laser-crystallized films, are investigated, featuring different photoexcited carrier and coherent optical phonon dynamics. At least two main phonon frequencies are identified for each phase/material and their evolution for increasing pump fluences is investigated for the fcc-crystalline phase and the laser-crystallized material, revealing strong differences. We find evidence that a considerable fraction of amorphous phase remains in the laser-crystallized material, which features a different phonon frequency, not related to other phases. These results are important for emerging strategies aimed at driving ultrafast phase transitions via coherent phonon excitation for applications in data storage. © 2011 American Institute of Physics.

V2O3 is the prototype system for the Mott transition, one of the most fundamental phenomena of electronic correlation. Temperature, doping or pressure induce a metal to insulator transition (MIT) between a paramagnetic metal (PM) and a paramagnetic insulator (PI). This or related MITs have a high technological potential, among others for intelligent windows and field effect transistors. However the spatial scale on which such transitions develop is not known in spite of their importance for research and applications. Here we unveil for the first time the MIT in Cr-doped V2O3 with submicron lateral resolution: with decreasing temperature, microscopic domains become metallic and coexist with an insulating background. This explains why the associated PM phase is actually a poor metal. The phase separation can be associated with a thermodynamic instability near the transition. This instability is reduced by pressure which drives a genuine Mott transition to an eventually homogeneous metallic state., Paper plus supplementary material

We investigate $\mathrm{Ba}({\mathrm{Fe}}_{0.65}{\mathrm{Ru}}_{0.35}{)}_{2}{\mathrm{As}}_{2}$, a compound in which superconductivity appears at the expense of magnetism, by transport measurements and angle resolved photoemission spectroscopy. By resolving the different Fermi surface pockets and deducing from their volumes the number of hole and electron carriers, we show that Ru induces neither hole nor electron doping. However, the Fermi surface pockets are about twice larger than in ${\mathrm{BaFe}}_{2}{\mathrm{As}}_{2}$. A change of sign of the Hall coefficient with decreasing temperature evidences the contribution of both carriers to the transport. Fermi velocities increase significantly with respect to ${\mathrm{BaFe}}_{2}{\mathrm{As}}_{2}$, suggesting a reduction of correlation effects.

The transient response of $\text{Ba}{({\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x})}_{2}{\text{As}}_{2}$, $x=0.08$ was studied by pump-probe optical reflectivity. After ultrafast photoexcitation, hot electrons were found to relax with two different characteristic times, indicating the presence of two distinct decay channels: a faster one, of less than 1 ps in the considered pump fluence range and a slower one, corresponding to lattice thermalization and lasting $\ensuremath{\cong}6\text{ }\text{ps}$. Our analysis indicates that the fast relaxation should be attributed to preferential scattering of the electrons with only a subset of the lattice-vibration modes with a second moment of the Eliashberg function $\ensuremath{\lambda}⟨{\ensuremath{\omega}}^{2}⟩\ensuremath{\cong}64\text{ }{\text{meV}}^{2}$. The simultaneous excitation of a strong fully symmetric ${A}_{1g}$ optical phonon corroborates this conclusion and makes it possible to deduce the value of $\ensuremath{\lambda}\ensuremath{\cong}0.12$. This small value for the electron-phonon coupling confirms that a phonon-mediated process cannot be the only mechanism leading to the formation of superconducting pairs in this family of pnictides.

We investigate Ba(Fe0.65Ru0.35)2As2, a compound in which superconductivity appears at the expense of magnetism, by transport measurements and angle resolved photoemission spectroscopy. By resolving the different Fermi surface pockets and deducing from their volumes the number of hole and electron carriers, we show that Ru induces neither hole nor electron doping. However, the Fermi surface pockets are about twice larger than in BaFe2As2. A change of sign of the Hall coefficient with decreasing temperature evidences the contribution of both carriers to the transport. Fermi velocities increase significantly with respect to BaFe2As2, suggesting a reduction of correlation effects.

The ultrafast response of the prototype Mott-Hubbard system (V1-xCrx)2O3 was systematically studied with fs pump-probe reflectivity, allowing us to clearly identify the effects of the metal-insulator transition on the transient response. The isostructural nature of the phase transition in this material made it possible to follow across the phase diagram the behaviour of the detected coherent acoustic wave, whose average value and lifetime depend on the thermodynamic phase and on the correlated electron density of states. It is also shown how coherent lattice oscillations can play an important role in some changes affecting the ultrafast electronic peak relaxation at the phase transition, changes which should not be mistakenly attributed to genuine electronic effects. These results clearly show that a thorough understanding of the ultrafast response of the material over several tenths of ps is necessary to correctly interpret its sub-ps excitation and relaxation regime, and appear to be of general interest also for other strongly correlated materials., Comment: 6 pages, 3 figures. Europhysics Letters (in press)

We report the observation of a coherent lattice oscillation in a pnictide superconductor. A coherent fully symmetric optical phonon was detected in $\text{Ba}{({\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x})}_{2}{\text{As}}_{2}$ ($x=0.06$ and $x=0.08$) using time-resolved pump-probe reflectivity with 40 fs time resolution. The analysis of the phonon parameters for various excitation fluences reveals no evident difference below and above the critical temperature, suggesting that the ${A}_{1g}$ mode is not involved in the superconducting phase transition.

We present a comprehensive angle-resolved photoemission study of the three-dimensional electronic structure of $\text{Ba}{({\text{Fe}}_{1\ensuremath{-}x}{\text{Co}}_{x})}_{2}{\text{As}}_{2}$. The wide range of dopings covered by this study, $x=0$ to $x=0.3$, allows to extract systematic features of the electronic structure. We show that there are three different hole pockets around the $\ensuremath{\Gamma}$ point: the two inner ones being nearly degenerate and rather two dimensional, the outer one presenting a strong three-dimensional character. The structure of the electron pockets is clarified by studying high doping contents, where they are enlarged. They are found to be essentially circular and two dimensional. From the size of the pockets, we deduce the number of holes and electrons present at the various dopings. We find that the net number of carriers is in good agreement with the bulk stoichiometry but that the number of each species (holes and electrons) is smaller than predicted by theory. Finally, we discuss the quality of nesting in the different regions of the phase diagram. The presence of the third hole pocket significantly weakens the nesting at $x=0$, so that it may not be a crucial ingredient in the formation of the spin-density wave. On the other hand, superconductivity seems to be favored by the coexistence of two-dimensional hole and electron pockets of similar sizes.

We present an angle resolved photoemission study of V2O3, a prototype system for the observation of Mott transitions in correlated materials. We show that the spectral features corresponding to the quasiparticle peak in the metallic phase present a marked wave vector dependence, with a stronger intensity along the GammaZ direction. The analysis of their intensity for different probing depths shows the existence of a characteristic length scale for the attenuation of coherent electronic excitations at the surface. This length scale, which is larger than the thickness of the surface region as normally defined for noncorrelated electronic states, is found to increase when approaching the Mott transition. These results are in agreement with the behavior of quasiparticles at surfaces as predicted by Borghi et al.

We present an angle resolved photoemission study of V2O3, a prototype system for the observation of Mott transitions in correlated materials. We show that the spectral features corresponding to the quasiparticle peak in the metallic phase present a marked wave vector dependence, with a stronger intensity along the GammaZ direction. The analysis of their intensity for different probing depths shows the existence of a characteristic length scale for the attenuation of coherent electronic excitations at the surface. This length scale, which is larger than the thickness of the surface region as normally defined for noncorrelated electronic states, is found to increase when approaching the Mott transition. These results are in agreement with the behavior of quasiparticles at surfaces as predicted by Borghi et al.

It has been recently demonstrated that a pump pulse can generate coherent charge fluctuations in a superconductor through a stimulated Raman process [Mansart, et al., Proc. Natl. Acad. Sci. USA 110, 4539 (2013)]. Here, we present a tutorial review of the basic phenomena involved and show how the technique bears a strong analogy with nuclear magnetic resonance and electron paramagnetic resonance. The reflectivity of the system gets modulated by the coherent charge fluctuation of the condensate. A resonance at the Mott scale allows to identify a high-energy excitation which is coupled to the superconducting quasiparticles.

Imaging of flux vortices in high quality MgB2 single crystals has been successfully performed in a commercial field-emission gun-based transmission electron microscope. In cryo-Lorentz microscopy, the sample quality and the vortex lattice can be monitored simultaneously, allowing one to relate microscopically the surface quality and the vortex dynamics. Such a vortex motion ultimately determines the flow resistivity rho(f), the knowledge of which is indispensable for practical applications such as superconducting magnets or wires for magnetic resonance imaging. The observed patterns have been analyzed and compared with other studies by cryo-Lorentz microscopy or Bitter decoration. We find that the vortex lattice arrangement depends strongly on the surface quality obtained during the specimen preparation, and tends to form a hexagonal Abrikosov lattice at a relatively low magnetic field. Stripes or gossamerlike patterns, recently suggested as potential signatures of an unconventional behavior of MgB2, were not observed.

Dynamical information on spin degrees of freedom of proteins or solids can be obtained by Nuclear Magnetic Resonance (NMR) and Electron Spin Resonance (ESR). A technique with similar versatility for charge degrees of freedom and their ultrafast correlations could move forward the understanding of systems like unconventional superconductors. By perturbing the superconducting state in a high-Tc cuprate using a femtosecond laser pulse, we generate coherent oscillations of the Cooper pair condensate which can be described by an NMR/ESR formalism. The oscillations are detected by transient broad-band reflectivity and found to resonate at the typical scale of Mott physics (2.6 eV), suggesting the existence of a non-retarded contribution to the pairing interaction, as in unconventional (non Migdal-Eliashberg) theories., Comment: Accepted for publication in the Proceedings of the National Academy of Sciences of the U.S.A. (PNAS)