Pulsewidth-switchable ultrafast source at 114 nm.

Femtosecond laser sources with high repetition rate in the ultraviolet (UV) and vacuum UV (VUV) are fundamental tools enabling tabletop time-resolved and angle-resolved photoemission spectroscopy in solids. We describe a VUV source at 114 nm (10.8 eV) based on an industrial grade ytterbium-doped ultrafast laser, a nonlinear pulse width selection stage, and two cascaded frequency tripling stages, first in crystals, second in xenon. The role of ionization in gas-based perturbative third harmonic generation phase-matching is analyzed using a simple theory, numerical simulations, and experimental data. The source features high photon flux, high repetition rate, and adjustable time resolutions. Thereby, in combination with a state-of-the-art angle-resolved photoemission spectroscopy (ARPES) apparatus it enables the study of the electronic dynamics of the whole Brillouin zone in a large number of materials.

Manipulating Dirac States in BaNiS2 by Surface Charge Doping.

In the Dirac semimetal BaNiS2, the Dirac nodes are located along the Γ-M symmetry line of the Brillouin zone, instead of being pinned at fixed high-symmetry points. We take advantage of this peculiar feature to demonstrate the possibility of moving the Dirac bands along the Γ-M symmetry line in reciprocal space by varying the concentration of K atoms adsorbed onto the surface of cleaved BaNiS2 single crystals. By means of first-principles calculations, we give a full account of this observation by considering the effect of the electrons donated by the K atom on the charge transfer gap, which establishes a promising tool for engineering Dirac states at surfaces, interfaces, and heterostructures.

Electron Dynamics in Hybrid Perovskites Reveal the Role of Organic Cations on the Screening of Local Charges.

The large tolerance of hybrid perovksites to the trapping of electrons by defects is a key asset in photovoltaic applications. Here, the ionic surface terminations of CH3NH3PbI3 are employed as a testbed to study the effect of electrostatic fields on the dynamics of excited carriers. We characterize the transition across the tetragonal to orthorhombic phase. The observed type II band offset and drift of the excited electrons highlight the important role that organic cations have on the screening of local electrostatic fields. When the orientation of organic cations is frozen in the orthorhombic phase, the positively charged termination induces a massive accumulation of excited electrons at the surface of the sample. Conversely, no electron accumulation is observed in the tetragonal phase. We conclude that the local fields cannot penetrate in the sample when the polarizability of freely moving cations boosts the dielectric constant up to ε = 120.

Moving Dirac nodes by chemical substitution.

Dirac fermions play a central role in the study of topological phases, for they can generate a variety of exotic states, such as Weyl semimetals and topological insulators. The control and manipulation of Dirac fermions constitute a fundamental step toward the realization of novel concepts of electronic devices and quantum computation. By means of Angle-Resolved Photo-Emission Spectroscopy (ARPES) experiments and ab initio simulations, here, we show that Dirac states can be effectively tuned by doping a transition metal sulfide, [Formula: see text], through Co/Ni substitution. The symmetry and chemical characteristics of this material, combined with the modification of the charge-transfer gap of [Formula: see text] across its phase diagram, lead to the formation of Dirac lines, whose position in k-space can be displaced along the [Formula: see text] symmetry direction and their form reshaped. Not only does the doping x tailor the location and shape of the Dirac bands, but it also controls the metal-insulator transition in the same compound, making [Formula: see text] a model system to functionalize Dirac materials by varying the strength of electron correlations.

Ultrafast dynamics of hot carriers in a quasi-two-dimensional electron gas on InSe.

Two-dimensional electron gases (2DEGs) are at the base of current nanoelectronics because of their exceptional mobilities. Often the accumulation layer forms at polar interfaces with longitudinal optical (LO) modes. In most cases, the many-body screening of the quasi-2DEGs dramatically reduces the Fröhlich scattering strength. Despite the effectiveness of such a process, it has been recurrently proposed that a remote coupling with LO phonons persists even at high carrier concentration. We address this issue by perturbing electrons in an accumulation layer via an ultrafast laser pulse and monitoring their relaxation via time- and momentum-resolved spectroscopy. The cooling rate of excited carriers is monitored at doping level spanning from the semiconducting to the metallic limit. We observe that screening of LO phonons is not as efficient as it would be in a strictly 2D system. The large discrepancy is due to the remote coupling of confined states with the bulk. Our data indicate that the effect of such a remote coupling can be mimicked by a 3D Fröhlich interaction with Thomas-Fermi screening. These conclusions are very general and should apply to field effect transistors (FET) with high-κ dielectric gates, van der Waals heterostructures, and metallic interfaces between insulating oxides.

Band Gap Renormalization, Carrier Multiplication, and Stark Broadening in Photoexcited Black Phosphorus.

We investigate black phosphorus by time- and angle-resolved photoelectron spectroscopy. The electrons excited by 1.57 eV photons relax down to a conduction band minimum within 1 ps. Despite the low band gap value, no relevant amount of carrier multiplication could be detected at an excitation density 3-6 × 1019 cm-3. In the thermalized state, the band gap renormalization is negligible up to a photoexcitation density that fills the conduction band by 150 meV. Astonishingly, a Stark broadening of the valence band takes place at an early delay time. We argue that electrons and holes with a high excess energy lead to inhomogeneous screening of near surface fields. As a consequence, the chemical potential is no longer pinned in a narrow impurity band.

Rashba coupling amplification by a staggered crystal field.

There has been increasing interest in materials where relativistic effects induce non-trivial electronic states with promise for spintronics applications. One example is the splitting of bands with opposite spin chirality produced by the Rashba spin-orbit coupling in asymmetric potentials. Sizable splittings have been hitherto obtained using either heavy elements, where this coupling is intrinsically strong, or large surface electric fields. Here by means of angular resolved photoemission spectroscopy and first-principles calculations, we give evidence of a large Rashba coupling of 0.25 eV Å, leading to a remarkable band splitting up to 0.15 eV with hidden spin-chiral polarization in centrosymmetric BaNiS2. This is explained by a huge staggered crystal field of 1.4 V Å(-1), produced by a gliding plane symmetry, that breaks inversion symmetry at the Ni site. This unexpected result in the absence of heavy elements demonstrates an effective mechanism of Rashba coupling amplification that may foster spin-orbit band engineering.

Stable topological insulators achieved using high energy electron beams.

Topological insulators are potentially transformative quantum solids with metallic surface states which have Dirac band structure and are immune to disorder. Ubiquitous charged bulk defects, however, pull the Fermi energy into the bulk bands, denying access to surface charge transport. Here we demonstrate that irradiation with swift (∼2.5 MeV energy) electron beams allows to compensate these defects, bring the Fermi level back into the bulk gap and reach the charge neutrality point (CNP). Controlling the beam fluence, we tune bulk conductivity from p- (hole-like) to n-type (electron-like), crossing the Dirac point and back, while preserving the Dirac energy dispersion. The CNP conductance has a two-dimensional character on the order of ten conductance quanta and reveals, both in Bi2Te3 and Bi2Se3, the presence of only two quantum channels corresponding to two topological surfaces. The intrinsic quantum transport of the topological states is accessible disregarding the bulk size.

Manipulating the Topological Interface by Molecular Adsorbates: Adsorption of Co-Phthalocyanine on Bi2Se3.

Topological insulators are a promising class of materials for applications in the field of spintronics. New perspectives in this field can arise from interfacing metal-organic molecules with the topological insulator spin-momentum locked surface states, which can be perturbed enhancing or suppressing spintronics-relevant properties such as spin coherence. Here we show results from an angle-resolved photemission spectroscopy (ARPES) and scanning tunnelling microscopy (STM) study of the prototypical cobalt phthalocyanine (CoPc)/Bi2Se3 interface. We demonstrate that that the hybrid interface can act on the topological protection of the surface and bury the Dirac cone below the first quintuple layer.

High-performance deep-ultraviolet optics for free-electron lasers.

Working with wavelengths shorter than the deep ultraviolet involves the development of dedicated optics for free-electron lasers with devoted coating techniques and characterizations. High-performance deep-ultraviolet optics are specially developed to create low-loss, high-reflectivity dielectric mirrors with long lifetimes in harsh synchrotron radiation environments. In February 2001, lasing at 189.7 nm, the shortest wavelength obtained so far with free-electron-laser oscillators, was obtained at the European Free-electron-laser project at ELETTRA Synchrotron Light Laboratory, Trieste, Italy. In July 2001, 330-mW extracted power at 250 nm was measured with optimized transmission mirrors. Research and development of coatings correlated to lasing performance are reported.