No Arabic abstract
By means of first principles calculations, we computed the effective electron-phonon coupling constant $G_0$ governing the electron cooling in photoexcited bismuth. $G_0$ strongly increases as a function of electron temperature, which can be traced back to the semi-metallic nature of bismuth. We also used a thermodynamical model to compute the time evolution of both electron and lattice temperatures following laser excitation. Thereby, we simulated the time evolution of (1 -1 0), (-2 1 1) and (2 -2 0) Bragg peak intensities measured by Sciaini et al [Nature 458, 56 (2009)] in femtosecond electron diffraction experiments. The effect of the electron temperature on the Debye-Waller factors through the softening of all optical modes across the whole Brillouin zone turns out to be crucial to reproduce the time evolution of these Bragg peak intensities.
We investigate the ultrafast response of the bismuth (111) surface by means of time resolved photoemission spectroscopy. The direct visualization of the electronic structure allows us to gain insights on electron-electron and electron-phonon interaction. Concerning electron-electron interaction, it is found that electron thermalization is fluence dependent and can take as much as several hundreds of femtoseconds at low fluences. This behavior is in qualitative agreement with Landaus theory of Fermi liquids but the data show deviations from the behavior of a common 3D degenerate electron gas. Concerning electron-phonon interaction, our data allows us to directly observe the coupling of individual Bloch state to the coherent $A_{1g}$ mode. It is found that surface states are much less coupled to this mode when compared to bulk states. This is confirmed by textit{ab initio} calculations of surface and bulk bismuth.
The Debye-Waller factor has been calculated for stabilized delta-phase plutonium with 5% aluminum. A quasi-harmonic Born-von Karman force model with temperature dependent phonon frequencies was used to calculate the mean-square thermal atomic displacement from absolute zero to 800 K. Implementation of the observed anomalous softening of the long wavelength phonons with increasing temperature cannot account for the softening of the measured thermal parameter at high temperatures nor for its rather high value at low temperatures. The implications for diffraction measurements on delta-phase stabilized plutonium alloys are discussed.
We determine experimentally the excited-state interatomic forces in photoexcited bismuth. The forces are obtained by a constrained least-squares fit of the excited-state dispersion obtained by femtosecond time-resolved x-ray diffuse scattering to a fifteen-nearest neighbor Born-von Karman model. We find that the observed softening of the zone-center $A_{1g}$ optical mode and transverse acoustic modes with photoexcitation are primarily due to a weakening of three nearest neighbor forces along the bonding direction. This provides a more complete picture of what drives the partial reversal of the Peierls distortion previously observed in photoexcited bismuth.
A new quantum-theoretical derivation of the elastic and inelastic scattering probability of He atoms from a metal surface, where the energy and momentum exchange with the phonon gas can only occur through the mediation of the surface free-electron density, shows that the Debye-Waller exponent is directly proportional to the electron-phonon mass coupling constant $lambda$. The comparison between the values of $lambda$ extracted from existing data on the Debye-Waller factor for various metal surfaces and the $lambda$ values known from literature indicates a substantial agreement, which opens the possibility of directly extracting the electron-phonon coupling strength in quasi-2D conducting systems from the temperature or incident energy dependence of the elastic Helium atom scattering intensities.
We report ultrafast surface pump and interface probe experiments on photoexcited carrier transport across single crystal bismuth films on sapphire. The film thickness is sufficient to separate carrier dynamics from lattice heating and strain, allowing us to investigate the time-scales of momentum relaxation, heat transfer to the lattice and electron-hole recombination. The measured electron-hole ($e-h$) recombination time is 12--26 ps and ambipolar diffusivity is 18--40 cm$^{2}$/s for carrier excitation up to $sim 10^{19} text{cm}^{-3}$. By comparing the heating of the front and back sides of the film, we put lower limits on the rate of heat transfer to the lattice, and by observing the decay of the plasma at the back of the film, we estimate the timescale of electron-hole recombination. We interpret each of these timescales within a common framework of electron-phonon scattering and find qualitative agreement between the various relaxation times observed. We find that the carrier density is not determined by the $e-h$ plasma temperature after a few picoseconds. The diffusion and recombination become nonlinear with initial excitation $gtrsim 10^{20} text{cm}^{-3}$.