No Arabic abstract
We performed terahertz time-domain spectroscopy, low-frequency Raman scattering, and Brillouin light scattering on vitreous glucose to investigate the boson peak (BP) dynamics. In the spectra of {alpha}({ u})/{ u}2 [{alpha}({ u}) is the absorption coefficient], the BP is clearly observed around 1.1 THz. Correspondingly, the complex dielectric constant spectra show a universal resonancelike behavior only below the BP frequency. As an analytical scheme, we propose the relative light-vibration coupling coefficient (RCC), which is obtainable from the combination of the far-infrared and Raman spectra. The RCC reveals that the infrared light-vibration coupling coefficient CIR({ u}) of the vitreous glucose behaves linearly on frequency which deviates from Taraskins model of CIR({ u}) = A + B{ u}2 [S. N. Taraskin et al., Phys. Rev. Lett. 97, 055504 (2006)]. The linearity of CIR({ u}) might require modification of the second term of the model. The measured transverse sound velocity shows an apparent discontinuity with the flattened mode observed in the inelastic neutron scattering study [N. Violini et al., Phys. Rev. B 85, 134204 (2012)] and suggests a coupling between the transverse acoustic and flattened modes.
Disordered systems exhibit universal excitation, referred to as the boson peak, in the terahertz region. Meanwhile, the so-called fracton is expected to appear in the nanoscale region owing to the self-similar structure of monomers in polymeric glasses. We demonstrate that such excitations can be detected using terahertz spectroscopy. For the interaction between terahertz light and the vibrational density of states of the fractal structure, we formulate an infrared light-vibration coupling coefficient for the fracton region. Accordingly, we show that information concerning fractal and fracton dimensions appears in the exponent of the absorption coefficient. Finally, using terahertz time-domain spectroscopy and low-frequency Raman scattering, we experimentally observe these universal excitations in a protein lysozyme system that has an intrinsically disordered and self-similar nature in a single supramolecule. These findings are applicable to disordered and polymeric glasses in general and will be key to understanding universal dynamics of disordered systems by terahertz light.
We present an angle-resolved photoemission spectroscopy study of the electronic structure of SnTe, and compare the experimental results to ab initio band structure calculations as well as a simplified tight-binding model of the p-bands. Our study reveals the conjectured complex Fermi surface structure near the L-points showing topological changes in the bands from disconnected pockets, to open tubes, and then to cuboids as the binding energy increases, resolving lingering issues about the electronic structure. The chemical potential at the crystal surface is found to be 0.5eV below the gap, corresponding to a carrier density of p =1.14x10^{21} cm^{-3} or 7.2x10^{-2} holes per unit cell. At a temperature below the cubic-rhombohedral structural transition a small shift in spectral energy of the valance band is found, in agreement with model predictions.
We investigated the photoexcited carrier dynamics in Si by using optical pump and terahertz probe spectroscopy in an energy range between 2 meV and 25 meV. The formation dynamics of excitons from unbound e-h pairs was studied through the emergence of the 1s-2p transition of excitons at 12 meV (3 THz). We revealed the thermalization mechanism of the photo-injected hot carriers (electrons and holes) in the low temperature lattice system by taking account of the interband and intraband scattering of carriers with acoustic and optical phonons. The overall cooling rate of electrons and holes was numerically calculated on the basis of a microscopic analysis of the phonon scattering processes, and the results well account for the experimentally observed carrier cooling dynamics. The long formation time of excitons in Si after the above-gap photoexcitation is reasonably accounted for by the thermalization process of photoexcited carriers.
We measure the anisotropic mid-infrared response of electrons and phonons in bulk YBa2Cu3O7 after femtosecond photoexcitation. A line shape analysis of specific lattice modes reveals their transient occupation and coupling to the superconducting condensate. The apex oxygen vibration is strongly excited within 150 fs demonstrating that the lattice absorbs a major portion of the pump energy before the quasiparticles are thermalized. Our results attest to substantial electron-phonon scattering and introduce a powerful concept probing electron-lattice interactions in a variety of complex materials.
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.