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International audience; Hybrid heterostructures, made of organic molecules adsorbed on two-dimensional metal monochalcogenide, generally unveil interfacial effects that improve the electronic properties of the single constitutive layers. Here, we investigate the interfacial electronic characteristics of the F4-TCNQ/single-layer GaSe heterostructure. A sharp F4-TCNQ/GaSe interface has been obtained and characterized by x-ray photoemission spectroscopy. We demonstrate that a high electron transfer from 1TL GaSe into the adsorbed F4-TCNQ molecules takes place, thereby yielding a reduction in the excess negative charge density of GaSe. Additionally, the direct band-structure determination of the heterostructure has been carried out using angle-resolved photoemission spectroscopy, shedding light on essential features such as doping and band offset at the interface. Our results indicate that the buried 1TL GaSe below the F4-TCNQ layer exhibits a robust inversion of the valence dispersion at the Γ point, forming a Mexican-hat-shaped dispersion with 120 ± 10 meV of depth. Our experiments also reveal that F4-TCNQ can significantly tune the electronic properties of 1TL GaSe by shifting the band offset of about 0.16 eV toward lower binding energies with respect to the Fermi level, which is a key feature for envisioning its applications in nanoelectronics.

Using femtosecond time- and angle-resolved photoemission spectroscopy, we explore the out-of-equilibrium dynamics of surface fermions in the topological system ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{2}\mathrm{Se}$. We show that the presence of localized states from defects at the surface is one of the key material parameters undergirding the long relaxation time of photoexcited Dirac electrons lying in the projected band gap of the bulk-insulating pristine compound. Doping this ternary compound with Sn substituting on Bi sites, while desirably increasing the resistivity at low temperatures decreases decay times of the excited homologous Dirac electrons. On the basis of these observations, we argue that long relaxation times can be ultimately controlled by a charge transfer to the surface.

We monitor the dynamics of hot carriers in InSe by means of two-photon photoelectron spectroscopy (2PPE). The electrons excited by photons of 3.12 eV experience a manifold relaxation. First, they thermalize to electronic states degenerate with the $\overline{M}$ valley. Subsequently, the electronic cooling is dictated by Fr\"ohlich coupling with phonons of small momentum transfer. Ab initio calculations predict cooling rates that are in good agreement with the observed dynamics. We argue that electrons accumulating in states degenerate with the $\overline{M}$ valley could travel through a multilayer flake of InSe with a lateral size of 1 $\ensuremath{\mu}\mathrm{m}$. The hot carriers pave a viable route to the realization of below-band-gap photodiodes and Gunn oscillators. Our results indicate that these technologies may find a natural implementation in future devices based on layered chalcogenides.

We address the role of nonlocal Coulomb correlations and short-range magnetic fluctuations in the high-temperature phase of ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$ within state-of-the-art spectroscopic and first-principles theoretical methods. Introducing an ``oriented-cluster dynamical mean-field scheme'', we compute momentum-resolved spectral functions, which we find to be in excellent agreement with angle-resolved photoemission spectra. We show that while short-range antiferromagnetic fluctuations are crucial to accounting for the electronic properties of ${\mathrm{Sr}}_{2}{\mathrm{IrO}}_{4}$ even in the high-temperature paramagnetic phase, long-range magnetic order is not a necessary ingredient of the insulating state. Upon doping, an exotic metallic state is generated, exhibiting cuprate-like pseudo-gap spectral properties, for which we propose a surprisingly simple theoretical mechanism.

We present a time- and angle-resolved photoemission study of the transition-metal dichalcogenide ${\mathrm{WTe}}_{2}$, a candidate type-II Weyl semimetal exhibiting extremely large magnetoresistence. Using femtosecond light pulses, we characterize the unoccupied states of the electron pockets above the Fermi level. Following the ultrafast carrier relaxation in distinct parts of the Brillouin zone, we report remarkably similar decay dynamics for electrons and holes. Our results confirm that charge compensation between electron and hole pockets---a key effect to explain the nonsaturating magnetoresistance of this material---is a distinctive feature of ${\mathrm{WTe}}_{2}$ even in an out-of-equilibrium regime.

We report time- and angle-resolved spectroscopic measurements in optimally doped ${\mathrm{Bi}}_{2}{\mathrm{Sr}}_{2}{\mathrm{CaCu}}_{2}{\mathrm{O}}_{8+\ensuremath{\delta}}$. The photoelectron intensity maps are monitored as a function of temperature, photoexcitation density, and delay time from the pump pulse. We evince that thermal fluctuations are effective only for temperatures near the critical value whereas photoinduced fluctuations scale linearly at low pumping fluence. The minimal energy to fully disrupt the superconducting gap slightly increases when moving off the nodal direction. No evidence of a pseudogap arising from other phenomena than pairing has been detected in the explored region of reciprocal space. On the other hand, a model accounting for the finite pair breaking explains the gap filling both in the near-nodal as well as in the off-nodal direction. Finally, we observed that nodal quasiparticles develop a faster dynamics when pumping the superconductor with fluence large enough to induce the total collapse of the gap.

We study with Angle Resolved PhotoElectron Spectroscopy (ARPES) the evolution of the electronic structure of Sr2IrO4, when holes or electrons are introduced, through Rh or La substitutions. At low dopings, the added carriers occupy the first available states, at bottom or top of the gap, revealing an anisotropic gap of 0.7eV in good agreement with STM measurements. At further doping, we observe a reduction of the gap and a transfer of spectral weight across the gap, although the quasiparticle weight remains very small. We discuss the origin of the in-gap spectral weight as a local distribution of gap values.

We perform time resolved photoelectron spectroscopy measurements of optimally doped $\tn{Bi}_2\tn{Sr}_2\tn{CaCu}_2\tn{O}_{8+\delta}$ (Bi-2212) and $\tn{Bi}_2\tn{Sr}_{2-x}\tn{La}_{x}\tn{Cu}\tn{O}_{6+\delta}$ (Bi-2201). The electrons dynamics show that inelastic scattering by nodal quasiparticles decreases when the temperature is lowered below the critical value of the superconducting phase transition. This drop of electronic dissipation is astonishingly robust and survives to photoexcitation densities much larger than the value sustained by long-range superconductivity. The unconventional behaviour of quasiparticle scattering is ascribed to superconducting correlations extending on a length scale comparable to the inelastic path. Our measurements indicate that strongly driven superconductors enter in a regime without phase coherence but finite pairing amplitude. The latter vanishes near to the critical temperature and has no evident link with the pseudogap observed by Angle Resolved Photoelectron Spectroscopy (ARPES)., Comment: 7 pages, 5 Figures

Time-resolved experiments visualize the motion of electrons in bilayer graphene, confirming the material behaves as a semiconductor that has potential for electronics applications.

Boron neutron capture therapy (BNCT) is an experimental, binary treatment for brain cancer which requires as the first step that tumor tissue is targeted with a boron-10 containing compound. Subsequent exposure to a thermal neutron flux results in destructive, short range nuclear reaction within 10 microm of the boron compound. The success of the therapy requires than the BNCT agents be well localized in tumor, rather than healthy tissue. The MEPHISTO spectromicroscope, which performs microchemical analysis by x-ray absorption near edge structure (XANES) spectroscopy from microscopic areas, has been used to study the distribution of trace quantities of boron in human brain cancer tissues surgically removed from patients first administered with the compound Na2B12H11SH (BSH). The interpretation of XANES spectra is complicated by interference from physiologically present sulfur and phosphorus, which contribute structure in the same energy range as boron. We addressed this problem with the present extensive set of spectra from S, B, and P in relevant compounds. We demonstrate that a linear combination of sulfate, phosphate and BSH XANES can be used to reproduce the spectra acquired on boron-treated human brain tumor tissues. We analyzed human glioblastoma tissue from two patients administered and one not administered with BSH. As well as weak signals attributed to BSH, x-ray absorption spectra acquired from tissue samples detected boron in a reduced chemical state with respect to boron in BSH. This chemical state was characterized by a sharp absorption peak at 188.3 eV. Complementary studies on BSH reference samples were not able to reproduce this chemical state of boron, indicating that it is not an artifact produced during sample preparation or x-ray exposure. These data demonstrate that the chemical state of BSH may be altered by in vivo metabolism.

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.

Ultrashort broadband terahertz pulses are applied to probe the electron dynamics of gaseous Ar and O-2 following ionization by an intense femtosecond laser pulse. The conductivity in the plasma center is extracted by a modified Wentzel-Kramers-Brillouin approach. It exhibits a nearly perfect Drude-like spectral shape and yields the temporal evolution of the free-electron density and collision rate. While the electron density in the Ar plasma remains nearly constant during the first 200 ps after generation, it decays much faster in O-2 due to dissociative recombination which is only possible in molecular plasmas. Adding a small amount of the electron scavenger SF6 to Ar reduces the electron lifetime in the plasma dramatically and allows us to determine the electron temperature to about 20 000 K. Furthermore, anomalously high, metal-like electron collision rates of up to 25 THz are found. Kinetic plasma theory substantially underestimates these rates pointing towards additional and more complex processes randomizing the total electronic momentum. Our results are relevant to both lightning control and generation of terahertz radiation by intense laser pulses in gases.

Time-resolved photoelectron spectroscopy is employed to study the dynamics of photoexcited electrons in optimally doped Bi{2}Sr{2}CaCu{2}O{8+delta} (Bi-2212). Hot electrons thermalize in less than 50 fs and dissipate their energy on two distinct time scales (110 fs and 2 ps). These are attributed to the generation and subsequent decay of nonequilibrium phonons, respectively. We conclude that 20% of the total lattice modes dominate the coupling strength and estimate the second momentum of the Eliashberg coupling function lambdaOmega{0}{2}=360+/-30 meV{2}. For the typical phonon energy of copper-oxygen bonds (Omega{0} approximately 40-70 meV), this results in an average electron-phonon coupling lambda

Femtosecond time-resolved photoemission is used to investigate the time evolution of electronic structure in the Mott insulator 1T-TaS2. A collapse of the electronic gap is observed within 100 femtoseconds after optical excitation. The photoemission spectra and the spectral function calculated by dynamical mean field theory show that this insulator-metal transition is driven solely by hot electrons. A coherently excited lattice displacement results in a periodic shift of the spectra lasting for 20 ps without perturbing the insulating phase. This capability to disentangle electronic and phononic excitations opens new directions to study electron correlation in solids.

Ultrafast charge carrier dynamics in graphite has been investigated by time-resolved terahertz spectroscopy. Analysis of the transient dielectric function and model calculations show that more than 90% of the initially deposited excitation energy is transferred to a few strongly coupled lattice vibrations within 500 fs. These hot optical phonons also substantially contribute to the striking increase of the Drude relaxation rate observed during the first picosecond after photoexcitation. The subsequent cooling of the hot phonons yields a lifetime estimate of 7 ps for these modes. Graphite has attracted continuous attention in research over the past decades [1]. Recently, a strong ambipolar electric field effect was found in thin films of this semimetal, thereby demonstrating its potential for future electronics [2]. Moreover, graphite is closely related to carbon nanotubes, which are the focus of nanotechnology research [3]. The latest experimental and theoretical efforts revealed that optical phonons in graphite strongly interact with the electrons [4,5]. These strongly coupled optical phonons (SCOPs) have high quantum energies of up to 0.2 eV and can be excited only by electrons of elevated energy. The scattering of electrons by SCOPsis believed to increase the dc resistivity of carbon nanotubes when high electric fields are applied [3]. In view of possible applications in electronics, further investigations are required on how SCOPs influence the transport and energy relaxation of electrons. Time-resolved terahertz spectroscopy (TRTS) is a promising experimental approach to this question. Avisible pump pulse excites charge carriers in the sample and thus enables them to generate optical phonons. A subsequent terahertz (THz) pulse probes the low-energy response of the system

High-resolution angle-resolved photoemission data from the insulating phase of the charge-density-wave (CDW) material 1T-TaS2 reveal the backfolding of the electronic bands associated with the CDW superlattice, but also an additional, unexpected periodicity. This periodicity is consistent with the dispersion predicted at zero temperature if three-sublattice magnetic order is present, suggesting that it is the signature of fluctuations associated with magnetic ordering of a Mott insulator on a triangular lattice.

We have measured the resonant inelastic x-ray scattering (RIXS) spectra at the Cu L3 edge in a variety of cuprates. Exploiting a considerably improved energy resolution (0.8 eV) we recorded significant dependencies on the sample composition and orientation, on the scattering geometry, and on the incident photon polarization. The RIXS final states correspond to two families of electronic excitations, having local (dd excitations) and nonlocal (charge-transfer) character. The dd energy splitting can be estimated with a simple crystal field model. The RIXS at the L3 edge demonstrates here a great potential, thanks to the resonance strength and to the large 2p spin-orbit splitting.

High-resolution angle-resolved photoemission data show that a metal-insulator Mott transition occurs at the surface of the quasi-two-dimensional compound 1T-TaSe2. The transition is driven by the narrowing of the Ta 5d band induced by a temperature-dependent modulation of the atomic positions. A dynamical mean-field theory calculation of the spectral function of the half-filled Hubbard model captures the main qualitative feature of the data, namely, the rapid transfer of spectral weight from the observed quasiparticle peak at the Fermi surface to the Hubbard bands, as the correlation gap opens up.

High-resolution angle-resolved photoemission spectroscopy (ARPES) on the quasi-one-dimensional Peierls system K0.3MoO3 reveals a "hidden" open Fermi surface and band features displaying the symmetry properties of the underlying lattice. However, the ARPES line shapes and optical data suggest that the corresponding quasiparticles are heavily renormalized by strong electron-phonon interactions. The temperature dependence of the leading edge of the mostly incoherent spectrum bears signatures of the Peierls transition at T-P=180 K and of pretransitional fluctuations.

Angle-resolved photoemission (ARPES) on the quasi-one-dimensional conductor (TaSe4)(2)I shows a hidden Fermi-surface crossing in its metallic state and the opening of a Peierls gap at low temperatures, The underlying quasiparticles have vanishing spectral weight and extremely short coherence lengths. They are interpreted as polarons in the strong-coupling adiabatic Lin-Lit, and almost all their ARPES weight is incoherent. These observations suggest a scenario where the long-standing contradictions between ARPES and other experiments on Peierls materials could be resolved.

We present a combined angle-resolved photoemission spectroscopy and resistivity study of the model Fermi liquid system 1T-TiTe2. From the analysis of the quasiparticle spectral line shape we identify and separately evaluate the electron-electron. electron-phonon, and impurity scattering contributions to the quasiparticle lifetime. There is a clear correspondence between spectroscopic and transport data. A residual low-temperature spectral linewidth (Gamma (o)=17 meV) indicates that the three-dimensional nature of the electronic states cannot be neglected even in this quasi-two-dimensional material.