Employing femtosecond laser pulses in front and back side pumping of Au/Fe/MgO(001) combined with detection in two-photon photoelectron emission spectroscopy we analyze local relaxation dynamics of excited electrons in buried Fe, injection into Au across the Fe-Au interface, and electron transport across the Au layer at 0.6 to 2.0 eV above the Fermi energy. By analysis as a function of Au film thickness we obtain the electron lifetimes of bulk Au and Fe and distinguish the relaxation in the heterostructures constituents. We also show that the excited electrons propagate through Au in a superdiffusive regime and conclude further that electron injection across the epitaxial interface proceeds ballistically by electron wavepacket propagation.
Based on results from femtosecond time-resolved photoemission, we compare three different methods for determination of the electron-phonon coupling constant {lambda} in Eu and Ba-based 122 FeAs compounds. We find good agreement between all three methods, which reveal a small {lambda} < 0.2. This makes simple electron-phonon mediated superconductivity unlikely in these compounds.
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 $pi$ 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.
We address local inelastic scattering from vibrational impurity adsorbed onto graphene and the evolution of the local density of electron states near the impurity from weak to strong coupling regime. For weak coupling the local electronic structure is distorted by inelastic scattering developing peaks/dips and steps. These features should be detectable in the inelastic electron tunneling spectroscopy, $d^2I/dV^2$, using local probing techniques. Inelastic Friedel oscillations distort the spectral density at energies close to the inelastic mode. In the strong coupling limit, a local negative $U$-center forms in the atoms surrounding the impurity site. For those atoms, the Dirac cone structure is fully destroyed, that is, the linear energy dispersion as well as the V-shaped local density of electron states is completely destroyed. We further consider the effects of the negative $U$ formation and its evolution from weak to strong coupling. The negative $U$-site effectively acts as local impurity such that sharp resonances appear in the local electronic structure. The main resonances are caused by elastic scattering off the impurity site, and the features are dressed by the presence of vibrationally activated side resonances. Going from weak to strong coupling, changes the local electronic structure from being Dirac cone like including midgap states, to a fully destroyed Dirac cone with only the impurity resonances remaining.
We characterize the topological insulator Bi$_2$Se$_3$ using time- and angle- resolved photoemission spectroscopy. By employing two-photon photoemission, a complete picture of the unoccupied electronic structure from the Fermi level up to the vacuum level is obtained. We demonstrate that the unoccupied states host a second, Dirac surface state which can be resonantly excited by 1.5 eV photons. We then study the ultrafast relaxation processes following optical excitation. We find that they culminate in a persistent non-equilibrium population of the first Dirac surface state, which is maintained by a meta-stable population of the bulk conduction band. Finally, we perform a temperature-dependent study of the electron-phonon scattering processes in the conduction band, and find the unexpected result that their rates decrease with increasing sample temperature. We develop a model of phonon emission and absorption from a population of electrons, and show that this counter-intuitive trend is the natural consequence of fundamental electron-phonon scattering processes. This analysis serves as an important reminder that the decay rates extracted by time-resolved photoemission are not in general equal to single electron scattering rates, but include contributions from filling and emptying processes from a continuum of states.
We demonstrate a novel method for the excitation of sizable magneto-optical effects in Au by means of the laser-induced injection of hot spin-polarized electrons in Au/Fe/MgO(001) heterostructures. It is based on the energy- and spin-dependent electron transmittance of Fe/Au interface which acts as a spin filter for non-thermalized electrons optically excited in Fe. We show that after crossing the interface, majority electrons propagate through the Au layer with the velocity on the order of 1 nm/fs (close to the Fermi velocity) and the decay length on the order of 100 nm. Featuring ultrafast functionality and requiring no strong external magnetic fields, spin injection results in a distinct magneto-optical response of Au. We develop a formalism based on the phase of the transient complex MOKE response and demonstrate its robustness in a plethora of experimental and theoretical MOKE studies on Au, including our ab initio calculations. Our work introduces a flexible tool to manipulate magneto-optical properties of metals on the femtosecond timescale that holds high potential for active magneto-photonics, plasmonics, and spintronics.