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Register a new userUltrafast Electron Dynamics in the Topological Insulator Bi2Se3 Studied by Time-Resolved Photoemission Spectroscopy
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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.
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We investigate the ultrafast transient absorption spectrum of Bi2Se3 topological insulator. Bi2Se3 single crystal is grown through conventional solid-state reaction routevia self-flux method. The structural properties have been studied in terms of high-resolution Powder X-ray Diffraction (PXRD). Detailed Rietveld analysis of PXRD of the crystal showed that sample is crystallized in the rhombohedral crystal structure with a space group of R-3m, and the lattice parameters are a=b=4.14A and c=28.7010A. Scanning Electron Microscopy (SEM) result shows perfectly crystalline structure with layered type morphology which evidenced from surface XRD. Energy Dispersive Spectroscopy (EDS) analysis determined quantitative amounts of the constituent atoms, found to be very close to their stoichiometric ratio. Further the fluence dependent nonlinear behaviour is studied by means of ultrafast transient absorption spectroscopy. The ultrafast spectroscopy also predicts the capability of this single crystal to generate Terahertz (THz) radiations (T-rays).
We report time- and angle-resolved photoemission spectroscopy measurements on the topological insulator Bi2Se3. We observe oscillatory modulations of the electronic structure of both the bulk and surface states at a frequency of 2.23 THz due to coherent excitation of an A1g phonon mode. A distinct, additional frequency of 2.05 THz is observed in the surface state only. The lower phonon frequency at the surface is attributed to the termination of the crystal and thus reduction of interlayer van der Waals forces, which serve as restorative forces for out-of-plane lattice distortions. DFT calculations quantitatively reproduce the magnitude of the surface phonon softening. These results represent the first band-resolved evidence of the A1g phonon mode coupling to the surface state in a topological insulator.
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.
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.
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.
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