M. Zacchigna

Direct view of hot carrier dynamics in graphene.

The ultrafast dynamics of excited carriers in graphene is closely linked to the Dirac spectrum and plays a central role for many electronic and optoelectronic applications. Harvesting energy from excited electron-hole pairs, for instance, is only possible if these pairs can be separated before they lose energy to vibrations, merely heating the lattice. Until now, the hot carrier dynamics in graphene could only be accessed indirectly. Here, we present a dynamical view on the Dirac cone by time- and angle-resolved photoemission spectroscopy. This allows us to show the quasi-instant thermalization of the electron gas to a temperature of ≈2000 K, to determine the time-resolved carrier density, and to disentangle the subsequent decay into excitations of optical phonons and acoustic phonons (directly and via supercollisions).

Ultrafast Dynamics of Massive Dirac Fermions in Bilayer Graphene

Bilayer graphene is a highly promising material for electronic and optoelectronic applications since it is supporting massive Dirac fermions with a tunable band gap. However, no consistent picture of the gaps effect on the optical and transport behavior has emerged so far, and it has been proposed that the insulating nature of the gap could be compromised by unavoidable structural defects, by topological in-gap states, or that the electronic structure could be altogether changed by many-body effects. Here, we directly follow the excited carriers in bilayer graphene on a femtosecond time scale, using ultrafast time- and angle-resolved photoemission. We find a behavior consistent with a single-particle band gap. Compared to monolayer graphene, the existence of this band gap leads to an increased carrier lifetime in the minimum of the lowest conduction band. This is in sharp contrast to the second substate of the conduction band, in which the excited electrons decay through fast, phonon-assisted interband transitions.

Ultrafast photodoping and effective Fermi-Dirac distribution of the Dirac particles in Bi2Se3

We exploit time- and angle-resolved photoemission spectroscopy to determine the evolution of the out-of-equilibrium electronic structure of the topological insulator Bi2Se3. The response of the Fermi-Dirac distribution to ultrashort IR laser pulses has been studied by modeling the dynamics of hot electrons after optical excitation. We disentangle a large increase in the effective temperature (T*) from a shift of the chemical potential (mu*), which is consequence of the ultrafast photodoping of the conduction band. The relaxation dynamics of T* and mu* are k independent and these two quantities uniquely define the evolution of the excited charge population. We observe that the energy dependence of the nonequilibrium charge population is solely determined by the analytical form of the effective Fermi-Dirac distribution.

Tunable Carrier Multiplication and Cooling in Graphene

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly (n-)doped graphene, we observe larger carrier multiplication factors (>3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less (p-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphenes dynamical response to a photoexcitation.

Polarized high-brilliance and high-resolution soft x-ray source at ELETTRA: The performance of beamline BACH

BACH, a soft x-ray beamline for polarization-dependent experiments at the Italian synchrotron radiation facility ELETTRA, was recently completed and characterized. Its performance, in terms of energy resolution, flux and polarization, is presented. Based on two APPLE II undulators, BACH covers the energy range between 35 and 1600 eV with the control of the light polarization. The monochromator is equipped with four gratings and allows one to work either in a high resolution or in a high flux mode. After the monochromator, the beamline is split into two branches with different refocusing properties. One is optimized to exploit the performance of the soft x-ray spectrometer (ComIXS) available at the beamline. Resolving powers between 12000 at 90 eV photon energy and 6600 near 867 eV were achieved using the high-resolution gratings and the smallest available slit width (10 μm). For the high-brilliance grating, which works between 290 and 1600 eV, resolving powers between 7000 at 400 eV and 2200 at 867 eV wer...

Evidence of reduced surface electron-phonon scattering in the conduction band of Bi2Se3 by nonequilibrium ARPES

The nature of the Dirac quasiparticles in topological insulators calls for a direct investigation of the electron-phonon scattering at the surface. By comparing time-resolved ARPES measurements of the topological insulator Bi2Se3 with different probing depths, we show that the relaxation dynamics of the electronic temperature of the conduction band is much slower at the surface than in the bulk. This observation suggests that surface phonons are less effective in cooling the electron gas in the conduction band.

Ultrafast Optical Control of the Electronic Properties of ZrTe5

We report on the temperature dependence of the ZrTe(5) electronic properties, studied at equilibrium and out of equilibrium, by means of time and angle resolved photoelectron spectroscopy. Our results unveil the dependence of the electronic band structure across the Fermi energy on the sample temperature. This finding is regarded as the dominant mechanism responsible for the anomalous resistivity observed at T*∼160  K along with the change of the charge carrier character from holelike to electronlike. Having addressed these long-lasting questions, we prove the possibility to control, at the ultrashort time scale, both the binding energy and the quasiparticle lifetime of the valence band. These experimental evidences pave the way for optically controlling the thermoelectric and magnetoelectric transport properties of ZrTe(5).

Momentum and photon energy dependence of the circular dichroic photoemission in the bulk Rashba semiconductors BiTeX (X = I, Br, Cl)

Bulk Rashba systems BiTeX (X = I, Br, Cl) are emerging as important candidates for developing spintronics devices because of the coexistence of spin-split bulk and surface states, along with the ambipolar character of the surface charge carriers. The need to study the spin texture of strongly spin-orbit-coupled materials has recently promoted circular dichroic angular resolved photoelectron spectroscopy (CD-ARPES) as an indirect tool to measure the spin and the angular degrees of freedom. Here we report a detailed photon-energy-dependent study of the CD-ARPES spectra in BiTeX (X = I, Br, Cl). Our work reveals a large variation in the magnitude and sign of the dichroism. Interestingly, we find that the dichroic signal modulates differently for the three compounds and for the different spin-split states. These findings show a momentum and photon-energy dependence for the CD-ARPES signals in the bulk Rashba semiconductor BiTeX (X = I, Br, Cl). Finally, the outcome of our experiment indicates the important relation between the modulation of the dichroism and the phase differences between the wave functions involved in the photoemission process. This phase difference can be due to initial- or final-state effects. In the former case the phase difference results in possible interference effects among the photoelectrons emitted from different atomic layers and characterized by entangled spin-orbital polarized bands. In the latter case the phase difference results from the relative phases of the expansion of the final state in different outgoing partial waves.

Ultrafast electron dynamics in epitaxial graphene investigated with time- and angle-resolved photoemission spectroscopy.

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the π band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

Resonant Raman x-ray scattering at the S 2p edge of iron pyrite

The x-ray absorption and resonant inelastic x-ray spectra of iron pyrite (FeS2) have been measured at the S 2p edge and compared with published electronic structure calculations. A minimum in the x-ray absorption intensity interpreted as indicating a gap in the unoccupied density of states is found from about 4 to 6 eV above the bottom of the conduction band, in agreement with some recent calculations. Resonant Raman scattering conditions were set up at the onset of S 2p3/2 absorption and a constant energy loss peak at 1.9 eV was observed. This is assigned to transitions from occupied tg to unoccupied eg states, both of which are predominantly of Fe 3d character but hybridized with the S valence states. This demonstrates that Fe dd excitations can be probed via S 2p resonant spectroscopy, as has been done recently at the O 1s edge for oxide materials.