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1.
Nat Commun ; 15(1): 4581, 2024 May 29.
Artigo em Inglês | MEDLINE | ID: mdl-38811546

RESUMO

The anomalous strange metal phase found in high-Tc cuprates does not follow the conventional condensed-matter principles enshrined in the Fermi liquid and presents a great challenge for theory. Highly precise experimental determination of the electronic self-energy can provide a test bed for theoretical models of strange metals, and angle-resolved photoemission can provide this as a function of frequency, momentum, temperature and doping. Here we show that constant energy cuts through the nodal spectral function in (Pb,Bi)2Sr2-xLaxCuO6+δ have a non-Lorentzian lineshape, consistent with a self-energy that is k dependent. This provides a new test for aspiring theories. Here we show that the experimental data are captured remarkably well by a power law with a k-dependent scaling exponent smoothly evolving with doping, a description that emerges naturally from anti-de Sitter/conformal-field-theory based semi-holography. This puts a spotlight on holographic methods for the quantitative modelling of strongly interacting quantum materials like the cuprate strange metals.

2.
Phys Rev Lett ; 131(23): 236502, 2023 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-38134803

RESUMO

We study the temperature evolution of quasiparticles in the correlated metal Sr_{2}RuO_{4}. Our angle resolved photoemission data show that quasiparticles persist up to temperatures above 200 K, far beyond the Fermi liquid regime. Extracting the quasiparticle self-energy, we demonstrate that the quasiparticle residue Z increases with increasing temperature. Quasiparticles eventually disappear on approaching the bad metal state of Sr_{2}RuO_{4} not by losing weight but via excessive broadening from super-Planckian scattering. We further show that the Fermi surface of Sr_{2}RuO_{4}-defined as the loci where the spectral function peaks-deflates with increasing temperature. These findings are in semiquantitative agreement with dynamical mean field theory calculations.

3.
Nat Commun ; 14(1): 7396, 2023 Nov 17.
Artigo em Inglês | MEDLINE | ID: mdl-37978297

RESUMO

Antiferromagnetic (AF) topological materials offer a fertile ground to explore a variety of quantum phenomena such as axion magnetoelectric dynamics and chiral Majorana fermions. To realize such intriguing states, it is essential to establish a direct link between electronic states and topology in the AF phase, whereas this has been challenging because of the lack of a suitable materials platform. Here we report the experimental realization of the AF topological-insulator phase in NdBi. By using micro-focused angle-resolved photoemission spectroscopy, we discovered contrasting surface electronic states for two types of AF domains; the surface having the out-of-plane component in the AF-ordering vector displays Dirac-cone states with a gigantic energy gap, whereas the surface parallel to the AF-ordering vector hosts gapless Dirac states despite the time-reversal-symmetry breaking. The present results establish an essential role of combined symmetry to protect massless Dirac fermions under the presence of AF order and widen opportunities to realize exotic phenomena utilizing AF topological materials.

4.
Phys Rev Lett ; 131(4): 046401, 2023 Jul 28.
Artigo em Inglês | MEDLINE | ID: mdl-37566843

RESUMO

The recent observation of correlated phases in transition metal dichalcogenide moiré systems at integer and fractional filling promises new insight into metal-insulator transitions and the unusual states of matter that can emerge near such transitions. Here, we combine real- and momentum-space mapping techniques to study moiré superlattice effects in 57.4° twisted WSe_{2} (tWSe_{2}). Our data reveal a split-off flat band that derives from the monolayer Γ states. Using advanced data analysis, we directly quantify the moiré potential from our data. We further demonstrate that the global valence band maximum in tWSe_{2} is close in energy to this flat band but derives from the monolayer K states which show weaker superlattice effects. These results constrain theoretical models and open the perspective that Γ-valley flat bands might be involved in the correlated physics of twisted WSe_{2}.

5.
Rev Sci Instrum ; 93(9): 093905, 2022 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-36182447

RESUMO

The APPLE-Knot undulator has been proposed to reduce the large on-axis heat load of the APPLE-II at very low photon energy. However, the current designs have an inherent non-zero second field integral due to the Knot sections, resulting in a transverse deflection of the electron beam throughout the undulator. For a long device, such a deviation can degrade the brightness and power distribution of the outgoing beam. Here, a new end-Knot section is presented to compensate for the electron trajectory, and the undulator is symmetrized to balance the output power distribution. The performance of the APPLE-Knot with symmetric power distribution is investigated. The partial power, flux, and polarization are compared with the APPLE-II. In the linear mode, APPLE-Knot shows a pronounced reduction of the partial power, with a similar flux to the APPLE-II. The symmetric power density distribution reduces the hotspot by 41%, with a flux loss of less than 5%. In the circular mode and at low photon energies, the flux is limited by the phase error of the symmetric design.

6.
Phys Rev Lett ; 126(17): 176403, 2021 Apr 30.
Artigo em Inglês | MEDLINE | ID: mdl-33988442

RESUMO

Using angle-resolved photoelectron spectroscopy (ARPES), we investigate the surface electronic structure of the magnetic van der Waals compounds MnBi_{4}Te_{7} and MnBi_{6}Te_{10}, the n=1 and 2 members of a modular (Bi_{2}Te_{3})_{n}(MnBi_{2}Te_{4}) series, which have attracted recent interest as intrinsic magnetic topological insulators. Combining circular dichroic, spin-resolved and photon-energy-dependent ARPES measurements with calculations based on density functional theory, we unveil complex momentum-dependent orbital and spin textures in the surface electronic structure and disentangle topological from trivial surface bands. We find that the Dirac-cone dispersion of the topologial surface state is strongly perturbed by hybridization with valence-band states for Bi_{2}Te_{3}-terminated surfaces but remains preserved for MnBi_{2}Te_{4}-terminated surfaces. Our results firmly establish the topologically nontrivial nature of these magnetic van der Waals materials and indicate that the possibility of realizing a quantized anomalous Hall conductivity depends on surface termination.

7.
Nat Commun ; 12(1): 2874, 2021 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-34001892

RESUMO

Topological superconductors (TSCs) are unconventional superconductors with bulk superconducting gap and in-gap Majorana states on the boundary that may be used as topological qubits for quantum computation. Despite their importance in both fundamental research and applications, natural TSCs are very rare. Here, combining state of the art synchrotron and laser-based angle-resolved photoemission spectroscopy, we investigated a stoichiometric transition metal dichalcogenide (TMD), 2M-WS2 with a superconducting transition temperature of 8.8 K (the highest among all TMDs in the natural form up to date) and observed distinctive topological surface states (TSSs). Furthermore, in the superconducting state, we found that the TSSs acquired a nodeless superconducting gap with similar magnitude as that of the bulk states. These discoveries not only evidence 2M-WS2 as an intrinsic TSC without the need of sensitive composition tuning or sophisticated heterostructures fabrication, but also provide an ideal platform for device applications thanks to its van der Waals layered structure.

8.
Phys Rev Lett ; 124(10): 106402, 2020 Mar 13.
Artigo em Inglês | MEDLINE | ID: mdl-32216410

RESUMO

We report high-resolution angle-resolved photoemission measurements on single crystals of Pt_{2}HgSe_{3} grown by high-pressure synthesis. Our data reveal a gapped Dirac nodal line whose (001) projection separates the surface Brillouin zone in topological and trivial areas. In the nontrivial k-space range, we find surface states with multiple saddle points in the dispersion, resulting in two van Hove singularities in the surface density of states. Based on density-functional theory calculations, we identify these surface states as signatures of a topological crystalline state, which coexists with a weak topological phase.

9.
Phys Chem Chem Phys ; 22(7): 3965-3974, 2020 Feb 19.
Artigo em Inglês | MEDLINE | ID: mdl-32022040

RESUMO

The photoelectron spectra of both liquid and gas phase aromatic molecules are reported. The spectra were obtained using a 34.1 eV source produced by high harmonic generation and analysed with the help of high-level ab initio simulations using the reflection principle combined with path integral molecular dynamics simulations accounting for nuclear quantum effects for the gas phase. We demonstrate the suitability of three trimethylbenzenes (1,3,5-trimethylbenzene, 1,2,3-trimethylbenzene and 1,2,4-trimethylbenzene) as a solvent for liquid photoelectron spectroscopy of solute species. We also discuss the electrokinetic charging of a non-polar liquid jet.

10.
Phys Rev E ; 100(4-1): 043207, 2019 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-31770899

RESUMO

The free-free opacity in dense systems is a property that both tests our fundamental understanding of correlated many-body systems, and is needed to understand the radiative properties of high energy-density plasmas. Despite its importance, predictive calculations of the free-free opacity remain challenging even in the condensed matter phase for simple metals. Here we show how the free-free opacity can be modelled at finite-temperatures via time-dependent density functional theory, and illustrate the importance of including local field corrections, core polarization, and self-energy corrections. Our calculations for ground-state Al are shown to agree well with experimental opacity measurements performed on the Artemis laser facility across a wide range of extreme ultraviolet wavelengths. We extend our calculations across the melt to the warm-dense matter regime, finding good agreement with advanced plasma models based on inverse bremsstrahlung at temperatures above 10 eV.

11.
Science ; 365(6459): 1282-1285, 2019 09 20.
Artigo em Inglês | MEDLINE | ID: mdl-31604236

RESUMO

Weyl semimetals are crystalline solids that host emergent relativistic Weyl fermions and have characteristic surface Fermi-arcs in their electronic structure. Weyl semimetals with broken time reversal symmetry are difficult to identify unambiguously. In this work, using angle-resolved photoemission spectroscopy, we visualized the electronic structure of the ferromagnetic crystal Co3Sn2S2 and discovered its characteristic surface Fermi-arcs and linear bulk band dispersions across the Weyl points. These results establish Co3Sn2S2 as a magnetic Weyl semimetal that may serve as a platform for realizing phenomena such as chiral magnetic effects, unusually large anomalous Hall effect and quantum anomalous Hall effect.

12.
Phys Rev Lett ; 121(7): 077205, 2018 Aug 17.
Artigo em Inglês | MEDLINE | ID: mdl-30169049

RESUMO

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 Fe_{3}O_{4} 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.

13.
Phys Rev Lett ; 118(13): 139902, 2017 Mar 31.
Artigo em Inglês | MEDLINE | ID: mdl-28409949

RESUMO

This corrects the article DOI: 10.1103/PhysRevLett.117.163002.

14.
Phys Rev Lett ; 117(16): 163002, 2016 Oct 14.
Artigo em Inglês | MEDLINE | ID: mdl-27792360

RESUMO

Hydrogen bonding interactions between biological chromophores and their surrounding protein and solvent environment significantly affect the photochemical pathways of the chromophore and its biological function. A common first step in the dynamics of these systems is excited state proton transfer between the noncovalently bound molecules, which stabilizes the system against dissociation and principally alters relaxation pathways. Despite such fundamental importance, studying excited state proton transfer across a hydrogen bond has proven difficult, leaving uncertainties about the mechanism. Through time-resolved photoelectron imaging measurements, we demonstrate how the addition of a single hydrogen bond and the opening of an excited state proton transfer channel dramatically changes the outcome of a photochemical reaction, from rapid dissociation in the isolated chromophore to efficient stabilization and ground state recovery in the hydrogen bonded case, and uncover the mechanism of excited state proton transfer at a hydrogen bond, which follows sequential hydrogen and charge transfer processes.

15.
Phys Rev Lett ; 117(27): 277201, 2016 Dec 30.
Artigo em Inglês | MEDLINE | ID: mdl-28084758

RESUMO

We report the spin-selective optical excitation of carriers in inversion-symmetric bulk samples of the transition metal dichalcogenide (TMDC) WSe_{2}. Employing time- and angle-resolved photoelectron spectroscopy (trARPES) and complementary time-dependent density functional theory (TDDFT), we observe spin-, valley-, and layer-polarized excited state populations upon excitation with circularly polarized pump pulses, followed by ultrafast (<100 fs) scattering of carriers towards the global minimum of the conduction band. TDDFT reveals the character of the conduction band, into which electrons are initially excited, to be two-dimensional and localized within individual layers, whereas at the minimum of the conduction band, states have a three-dimensional character, facilitating interlayer charge transfer. These results establish the optical control of coupled spin-, valley-, and layer-polarized states in centrosymmetric materials with locally broken symmetries and suggest the suitability of TMDC multilayer and heterostructure materials for valleytronic and spintronic device concepts.

16.
Phys Rev Lett ; 115(8): 086803, 2015 Aug 21.
Artigo em Inglês | MEDLINE | ID: mdl-26340199

RESUMO

Direct and inverse Auger scattering are amongst the primary processes that mediate the thermalization of hot carriers in semiconductors. These two processes involve the annihilation or generation of an electron-hole pair by exchanging energy with a third carrier, which is either accelerated or decelerated. Inverse Auger scattering is generally suppressed, as the decelerated carriers must have excess energies higher than the band gap itself. In graphene, which is gapless, inverse Auger scattering is, instead, predicted to be dominant at the earliest time delays. Here, <8 fs extreme-ultraviolet pulses are used to detect this imbalance, tracking both the number of excited electrons and their kinetic energy with time-and angle-resolved photoemission spectroscopy. Over a time window of approximately 25 fs after absorption of the pump pulse, we observe an increase in conduction band carrier density and a simultaneous decrease of the average carrier kinetic energy, revealing that relaxation is in fact dominated by inverse Auger scattering. Measurements of carrier scattering at extreme time scales by photoemission will serve as a guide to ultrafast control of electronic properties in solids for petahertz electronics.

17.
Phys Rev Lett ; 114(9): 097401, 2015 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-25793848

RESUMO

The prospect of optically inducing and controlling a spin-polarized current in spintronic devices has generated wide interest in the out-of-equilibrium electronic and spin structure of topological insulators. In this Letter we show that only measuring the spin intensity signal over several orders of magnitude by spin-, time-, and angle-resolved photoemission spectroscopy can provide a comprehensive description of the optically excited electronic states in Bi_{2}Se_{3}. Our experiments reveal the existence of a surface resonance state in the second bulk band gap that is benchmarked by fully relativistic ab initio spin-resolved photoemission calculations. We propose that the newly reported state plays a major role in the ultrafast dynamics of the system, acting as a bottleneck for the interaction between the topologically protected surface state and the bulk conduction band. In fact, the spin-polarization dynamics in momentum space show that these states display macroscopically different temperatures and, more importantly, different cooling rates over several picoseconds.

18.
Rev Sci Instrum ; 85(10): 103117, 2014 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-25362381

RESUMO

We present a simple electron time of flight spectrometer for time resolved photoelectron spectroscopy of liquid samples using a vacuum ultraviolet (VUV) source produced by high-harmonic generation. The field free spectrometer coupled with the time-preserving monochromator for the VUV at the Artemis facility of the Rutherford Appleton Laboratory achieves an energy resolution of 0.65 eV at 40 eV with a sub 100 fs temporal resolution. A key feature of the design is a differentially pumped drift tube allowing a microliquid jet to be aligned and started at ambient atmosphere while preserving a pressure of 10(-1) mbar at the micro channel plate detector. The pumping requirements for photoelectron (PE) spectroscopy in vacuum are presented, while the instrument performance is demonstrated with PE spectra of salt solutions in water. The capability of the instrument for time resolved measurements is demonstrated by observing the ultrafast (50 fs) vibrational excitation of water leading to temporary proton transfer.


Assuntos
Espectroscopia Fotoeletrônica/instrumentação , Soluções/química , Raios Ultravioleta , Vácuo , Calibragem , Desenho de Equipamento , Fatores de Tempo
19.
Environ Sci Pollut Res Int ; 20(4): 1937-50, 2013 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-23322412

RESUMO

In 2009, hexachlorocyclohexane (HCH) isomers (α-HCH, ß-HCH, and γ-HCH [lindane]) were listed as persistent organic pollutants (POP) in the Stockholm Convention. Accordingly, the legacy of HCH/lindane production with the associated large HCH waste deposits has become recognized as an issue of global concern and is addressed in the implementation of the Convention. The current paper gives an overview of the major contaminated sites from lindane production of the INQUINOSA Company. This company operated from 1975 to 1988 in the city of Sabiñánigo, Spain. HCH production resulted in the production of approximately 115,000 tonnes of waste isomers which were mainly dumped in two unlined landfills. These two landfill sites, together with the former production site, are recognized sources of environmental pollution. Assessment and remediation activities at these sites are described. A dense nonaqueous phase liquid (DNAPL) contaminated inter alia with HCH isomers, benzene, chlorobenzenes, and chlorophenols as the main contaminants and an associated contaminated groundwater plume have been discovered at both landfill/dumpsites and at the former production site. The approximately 4,000 t of DNAPLs constitute a serious risk for the environment due to the proximity of the Gállego River. Since 2004, more than 20 tonnes of this DNAPL has been extracted using "pump and treat" techniques. The Aragon Regional Government and the Spanish Environmental Ministry are taking action, focusing on the treatment of DNAPL and on the transfer of the large quantities of solid POP wastes to a new landfill. A range of laboratory tests has been performed in order to plan the aquifer remediation.


Assuntos
Monitoramento Ambiental/métodos , Recuperação e Remediação Ambiental/métodos , Resíduos Perigosos/análise , Hexaclorocicloexano/análise , Resíduos Industriais/análise , Resíduos de Praguicidas/análise , Indústria Química , Monitoramento Ambiental/economia , Recuperação e Remediação Ambiental/economia , Hidrologia , Modelos Teóricos , Espanha , Poluentes Químicos da Água/análise , Poluição Química da Água/análise , Poluição Química da Água/prevenção & controle
20.
Phys Chem Chem Phys ; 14(18): 6289-97, 2012 May 14.
Artigo em Inglês | MEDLINE | ID: mdl-22322861

RESUMO

Laser induced acoustic desorption (LIAD) has been used for the first time to study the parent ion production and fragmentation mechanisms of a biological molecule in an intense femtosecond (fs) laser field. The photoacoustic shock wave generated in the analyte substrate (thin Ta foil) has been simulated using the hydrodynamic HYADES code, and the full LIAD process has been experimentally characterised as a function of the desorption UV-laser pulse parameters. Observed neutral plumes of densities >10(9) cm(-3) which are free from solvent or matrix contamination demonstrate the suitability and potential of the source for studying ultrafast dynamics in the gas phase using fs laser pulses. Results obtained with phenylalanine show that through manipulation of fundamental femtosecond laser parameters (such as pulse length, intensity and wavelength), energy deposition within the molecule can be controlled to allow enhancement of parent ion production or generation of characteristic fragmentation patterns. In particular by reducing the pulse length to a timescale equivalent to the fastest vibrational periods in the molecule, we demonstrate how fragmentation of the molecule can be minimised whilst maintaining a high ionisation efficiency.


Assuntos
Acústica , Gases/química , Lasers , Fenilalanina/química , Temperatura , Cinética , Tantálio/química
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