The study of photoexcited strongly correlated materials is attracting growing interest since their rich phase diagram often translates into an equally rich out-of-equilibrium behaviour. With femtosecond optical pulses, electronic and lattice degrees of freedom can be transiently decoupled, giving the opportunity of stabilizing new states inaccessible by quasi-adiabatic pathways. Here we show that the prototype Mott–Hubbard material V2O3 presents a transient non-thermal phase developing immediately after ultrafast photoexcitation and lasting few picoseconds. For both the insulating and the metallic phase, the formation of the transient configuration is triggered by the excitation of electrons into the bonding a1g orbital, and is then stabilized by a lattice distortion characterized by a hardening of the A1g coherent phonon, in stark contrast with the softening observed upon heating. Our results show the importance of selective electron–lattice interplay for the ultrafast control of material parameters, and are relevant for the optical manipulation of strongly correlated systems.
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, BaNiS2, through Co/Ni substitution. The symmetry and chemical characteristics of this material, combined with the modification of the charge-transfer gap of BaCo1−xNixS2 across its phase diagram, lead to the formation of Dirac lines, whose position in k-space can be displaced along the Γ−M 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 BaCo1−xNixS2 a model system to functionalize Dirac materials by varying the strength of electron correlations.
We present a time-and angular-resolved photoemission (TR-ARPES) study of the transitionmetal dichalcogenide WTe2, 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 non saturating magnetoresistance of this material-is a distinctive feature of WTe2 even in an out-of-equilibrium regime.
We present an experimental study describing the effects of surface termination on the electronic structure of the natural topological superlattice phase Sb2Te. Using scanning angle-resolved photoemission microscopy, we consistently find various non-equivalent regions on the same surface after cleaving various Sb2Te single crystals. We were able to identify three distinct terminations characterized by different Sb/Te surface stoichiometric ratios and with clear differences in their band structure. For the dominating Te-rich termination, we also provide a direct observation of the excited electronic states and of their relaxation dynamics by means of time-resolved angle-resolved photoemission spectroscopy. Our results clearly indicate that the surface electronic structure is strongly affected by the bulk properties of the superlattice.
We demonstrate a table-top source delivering ultra-broadband THz pulses with electric field strength exceeding 100 kV/cm at a repetition rate of 200 kHz. The source is based on optical rectification of 23 fs pulses at 1030 nm delivered by a ytterbium-doped fiber laser followed by a nonlinear temporal compression stage. We generate THz pulses with a conversion efficiency of up to 0.11 % with a spectrum extending to 11 THz using a 1 mm thick GaP crystal and a conversion efficiency of 0.016 % with a spectrum extending to 30 THz using a 30 µm thick GaSe crystal. The essential features of the emitted THz pulse spectra are well captured by simulations of the optical rectification process relying on coupled nonlinear equations. Our ultrafast laser-based source uniquely satisfies an important requirement of nonlinear THz experiments, namely the emission of ultra-broadband THz pulses with high electric field amplitudes at high repetition rates, opening a route towards nonlinear time-resolved THz experiments with high signal-to-noise ratios.
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