No Arabic abstract
We describe a theoretical approach for spin-polarized hot-electron transport, as it occurs after excitation by ultrafast optical pulses in heterostructures formed by ferromagnetic and normal metals. We formulate a spin-dependent particle-in-cell model that solves the Boltzmann equation for excited electrons. It includes lifetimes and transmission coefficients as parameters, which can be taken from ab-initio calculations or experiment, and can be easily extended to multilayer systems. This approach is capable of describing electron transport in the ballistic, super-diffusive and diffusive regime including secondary-carrier generation. We apply the model to optically excited carriers in Fe/Au bilayers and Fe/Au/Fe spin-valve structures. We gain microscopic insight into the hot-electron transport dynamics probed in recent experiments on spin-valves. We find contributions to the demagnetization dynamics induced in Fe/Au/Fe trilayers regardless of the parallel or antiparallel magnetic alignment of the Fe layers.
We monitor the dynamics of hot carriers in InSe by means of two photons photoelectron spectroscopy (2PPE). The electrons excited by photons of 3.12 eV experience a manifold relaxation. First, they thermalize to the electronic states degenerate with the $bar M$ valley. Subsequently, the electronic cooling is dictated by Frohlich coupling with phonons of small momentum transfer. Ab-initio calculations predict cooling rates that are in good agreement with the observed dynamics. We argue that electrons accumulating in states degenerate with the $bar M$ valley could travel through a multilayer flake of InSe with lateral size of 1 micrometer. The hot carriers pave a viable route to the realization of below-bandgap photodiodes and Gunn oscillators. Our results indicate that these technologies may find a natural implementation in future devices based on layered chalcogenides.
Ultrafast time-resolved differential reflectivity of Bi2Se3 crystals is studied using optical pump-probe spectroscopy. Three distinct relaxation processes are found to contribute to the initial transient reflectivity changes. The deduced relaxation timescale and the sign of the reflectivity change suggest that electron-phonon interactions and defect-induced charge trapping are the underlying mechanisms for the three processes. After the crystal is exposed to air, the relative strength of these processes is altered and becomes strongly dependent on the excitation photon energy.
We discuss the ultrafast evolution of the surface electronic structure of the topological insulator Bi$_2$Te$_3$ following a femtosecond laser excitation. Using time and angle resolved photoelectron spectroscopy, we provide a direct real-time visualisation of the transient carrier population of both the surface states and the bulk conduction band. We find that the thermalization of the surface states is initially determined by interband scattering from the bulk conduction band, lasting for about 0.5 ps; subsequently, few ps are necessary for the Dirac cone non-equilibrium electrons to recover a Fermi-Dirac distribution, while their relaxation extends over more than 10 ps. The surface sensitivity of our measurements makes it possible to estimate the range of the bulk-surface interband scattering channel, indicating that the process is effective over a distance of 5 nm or less. This establishes a correlation between the nanoscale thickness of the bulk charge reservoir and the evolution of the ultrafast carrier dynamics in the surface Dirac cone.
Heterostructures of atomically thin van der Waals bonded monolayers have opened a unique platform to engineer Coulomb correlations, shaping excitonic, Mott insulating, or superconducting phases. In transition metal dichalcogenide heterostructures, electrons and holes residing in different monolayers can bind into spatially indirect excitons with a strong potential for optoelectronics, valleytronics, Bose condensation, superfluidity, and moire-induced nanodot lattices. Yet these ideas require a microscopic understanding of the formation, dissociation, and thermalization dynamics of correlations including ultrafast phase transitions. Here we introduce a direct ultrafast access to Coulomb correlations between monolayers; phase-locked mid-infrared pulses allow us to measure the binding energy of interlayer excitons in WSe2/WS2 hetero-bilayers by revealing a novel 1s-2p resonance, explained by a fully quantum mechanical model. Furthermore, we trace, with subcycle time resolution, the transformation of an exciton gas photogenerated in the WSe2 layer directly into interlayer excitons. Depending on the stacking angle, intra- and interlayer species coexist on picosecond scales and the 1s-2p resonance becomes renormalized. Our work provides a direct measurement of the binding energy of interlayer excitons and opens the possibility to trace and control correlations in novel artificial materials.
Trigonal tellurium (Te) is a chiral semiconductor that lacks both mirror and inversion symmetries, resulting in complex band structures with Weyl crossings and unique spin textures. Detailed time-resolved polarized reflectance spectroscopy is used to investigate its band structure and carrier dynamics. The polarized transient spectra reveal optical transitions between the uppermost spin-split H4 and H5 and the degenerate H6 valence bands (VB) and the lowest degenerate H6 conduction band (CB) as well as a higher energy transition at the L-point. Surprisingly, the degeneracy of the H6 CB (a proposed Weyl node) is lifted and the spin-split VB gap is reduced upon photoexcitation before relaxing to equilibrium as the carriers decay. Using ab initio density functional theory (DFT) calculations we conclude that the dynamic band structure is caused by a photoinduced shear strain in the Te film that breaks the screw symmetry of the crystal. The band-edge anisotropy is also reflected in the hot carrier decay rate, which is a factor of two slower along c-axis than perpendicular to it. The majority of photoexcited carriers near the band-edge are seen to recombine within 30 ps while higher lying transitions observed near 1.2 eV appear to have substantially longer lifetimes, potentially due to contributions of intervalley processes in the recombination rate. These new findings shed light on the strong correlation between photoinduced carriers and electronic structure in anisotropic crystals, which opens a potential pathway for designing novel Te-based devices that take advantage of the topological structures as well as strong spin-related properties.