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Register a new userUnraveling photoinduced spin dynamics in topological insulator Bi2Se3
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We report on time-resolved ultrafast optical spectroscopy study of the topological insulator (TI) Bi$_2$Se$_3$. We unravel that a net spin polarization can not only be generated using circularly polarized light via interband transitions between topological surface states (SSs), but also via transitions between SSs and bulk states. Our experiment demonstrates that tuning photon energy or temperature can essentially allow for photoexcitation of spin-polarized electrons to unoccupied topological SSs with two distinct spin relaxation times ($sim$25 fs and $sim$300 fs), depending on the coupling between SSs and bulk states. The intrinsic mechanism leading to such distinctive spin dynamics is the scattering in SSs and bulk states which is dominated by $E_g^2$ and $A_{1g}^1$ phonon modes, respectively. These findings are suggestive of novel ways to manipulate the photoinduced coherent spins in TIs.
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We study the manipulation of the photoelectron spin-polarization in Bi$_2$Se$_3$ by spin- and angle-resolved photoemission spectroscopy. General rules are established that enable controlling the spin-polarization of photoemitted electrons via light polarization, sample orientation, and photon energy. We demonstrate the $pm$100% reversal of a single component of the measured spin-polarization vector upon the rotation of light polarization, as well as a full three-dimensional manipulation by varying experimental configuration and photon energy. While a material-specific density-functional theory analysis is needed for the quantitative description, a minimal two-atomic-layer model qualitatively accounts for the spin response based on the interplay of optical selection rules, photoelectron interference, and topological surface-state complex structure. It follows that photoelectron spin-polarization control is generically achievable in systems with a layer-dependent, entangled spin-orbital texture.
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).
The nonlinear Hall effect due to Berry curvature dipole (BCD) induces frequency doubling, which was recently observed in time-reversal-invariant materials. Here we report novel electric frequency doubling in the absence of BCD on a surface of the topological insulator Bi2Se3 under zero magnetic field. We observe that the frequency-doubling voltage transverse to the applied ac current shows a threefold rotational symmetry, whereas it forbids BCD. One of the mechanisms compatible with the symmetry is skew scattering, arising from the inherent chirality of the topological surface state. We introduce the Berry curvature triple, a high-order moment of the Berry curvature, to explain skew scattering under the threefold rotational symmetry. Our work paves the way to obtain a giant second-order nonlinear electric effect in high mobility quantum materials, as the skew scattering surpasses other mechanisms in the clean limit.
We present a magneto-infrared spectroscopic study of thin Bi2Se3 single crystal flakes. Magneto-infrared transmittance and reflectance measurements are performed in the Faraday geometry at 4.2K in a magnetic field up to 17.5T. Thin Bi2Se3 flakes (much less than 1{mu}m thick) are stabilized on the Scotch tape, and the reduced thickness enables us to obtain appreciable far-infrared transmission through the highly reflective Bi2Se3 single crystals. A pronounced electron-phonon coupling is manifested as a Fano resonance at the {alpha} optical phonon mode in Bi2Se3, resulting from the quantum interference between the optical phonon mode and the continuum of the electronic states. However, the Fano resonance exhibits no systematic line broadening, in contrast to the earlier observation of a similar Fano resonance in Bi2Se3 using magneto-infrared reflectance spectroscopy.
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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