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As demonstrated with SPA-LEED and STM uniform height islands of preferred thickness form during the growth of Pb on Si(111). The islands form at temperatures T<250K and for fluxes F 1/60ML/sec which requires fast kinetics and balance between several atomic processes: diffusion towards the islands , diffusion to higher layers and preference for the atoms to remain on top of the preferred height islands. We have carried out SPA-LEED experiments to measure the barriers of the processes: we prepare an initial predominantly 5-step island height distribution and we deposit an additional 0.5ML Pb at different growth temperatures Tg to determine the transition to the next preferred height of 7-step islands (i.e. 2-step islands on top of the 5-step islands) with Spot Profile Analysis(SPA-LEED). We observe that 7-step island formation is possible above a minimum temperature Tg*=175K which indicates that the transfer of atoms from the surrounding region to the top of the islands is the main controlling process.
While surface kinetics measurements for single atom diffusion have proliferated, little work exists attempting to measure surface dynamics under equilibrium conditions. We will present our recent work on developing Temporal LEED Spectroscopy (TLS) as a dynamic probe of surfaces capable of kinetics measurements at both high temperatures and surface coverages. By tuning the diffraction to specific structural entities such as steps, islands, etc., and monitoring the diffracted signal as a function of time, dynamics information about these structures can be obtained. As an example we will present TLS results for the dynamics of step fluctuations on Si(001) [1]. We have measured activation energies and identified step-edge diffusion as the rate limiting process for 950K < T < 1130K. Although this result is in apparent disagreement with earlier work, a careful analysis, considering crossover temperatures between different microscopic processes, can reconcile the differences. 1. M. Kammler, et al., Phys. Rev. B (in press).
We present the first demonstration of Temporal LEED Spectroscopy’s ability to measure surface dynamics as shown by a study of step dynamics on vicinal Si(001). While we measure activation energies consistent with other work, the observed microscopic mechanism driving the fluctuations is inconsistent with previous claims. We exclude evaporation/condensation of atoms from the steps as the rate limiting kinetics in the temperature range of this experiment. Possible reasons for these differences are discussed.
Ultrafast X-ray diffraction
(2004)
Many fundamental processes in solids, such as heat transport and phase transitions involve atomic movement on ultrafast time-scales, but cannot be directly measured with visible light. Using ultrafast x-ray diffraction, atomic motion can be measured on its natural time-scale. Photo-excitation of bulk and layered semiconductors was achieved with 800-nm wavelength femtosecond laser pulses. Optical excitation triggers a chain of relaxation processes, causing rapid lattice heating, generation and propagation of stress/strain waves into the bulk and eventual anharmonic decay of coherent acoustic phonons into the thermal bath of the solid. While the first steps of carrier relaxation, excitation and decay of Raman-active optical phonons have been in the past characterized optically at surfaces, the bulk acoustic dynamics at longer times has not. We measure length scales of lattice excitation, thereby detecting ultrafast heat diffusion via fast electrons, coherent acoustic pulse propagation into the bulk or across buried interfaces and anharmonic damping of non-equilibrium acoustic phonons. The measurement is performed with sensitivity on lattice spacing of 10 femtometers (i.e., 3 nuclear diameters).
Many fundamental processes in nature, such as chemical reactions and phase transitions involve rearrangement of the constituent atoms. Such changes cannot be directly measured with visible light and occur transiently on time-scales comparable with the natural oscillation periods of atoms (femtoseconds to picoseconds). We present experiments on Ge-111 films irradiated with 100-fs 800-nm light pulses and probed by a time-delayed sub-ps x-ray pulse at 8 keV. After excitation of a dense electron-hole plasma within the 160-nm film, the ultrafast pathway of lattice disordering is measured as a function laser fluence. For close-to-threshold irradiation, inhomogeneous thermal melting, occurring via surface nucleation of the liquid phase and growth into the bulk determines the dynamics of the solid-to-liquid phase transition. For excitation at about twice the melting threshold, a nonthermal pathway, starting from a highly excited cold solid and relaxing into a hot liquid causes ultrafast melting. At long time delays, nearly perfect recrystallization of a (111) crystal is observed.
Summary form only given. Ultrashort x-ray pulses offer a unique combination of atomic-scale spatial and temporal resolution, which permits direct measurements of structural transients on an ultrafast time scale. Using time-resolved X-ray diffraction with femtosecond, multi-keV X-ray pulses we have studied transient lattice dynamics in optically excited semiconductors.
Summary form only given, as follow. Ultrafast optical-pump, X-ray diffraction probe experiments are providing new ways to study transient processes including the direct observation of the atomic motion by which many solid-state processes and chemical and biochemical reactions take place. Current table-top-terawatt femtosecond laser systems provide an attractive source of few-hundred femtosecond duration bursts of angstrom-scale X-ray radiation with fluxes comparable to standard rotating anode sources. Their compact size enables time resolved structural dynamics to be studied in the small laboratory with temporal resolution better than typical molecular vibrational periods. Ultrafast structural dynamics in crystalline samples are readily studied with such systems and experiments to be discussed in this talk include ultrafast non-thermal solid-to-liquid transition in thin single-crystal Ge-111 films grown on Si-111 substrates; ultrafast non-thermal solid-to-solid transitions in bulk vanadium dioxide from a low temperature insulating phase to a high temperature metallic phase; and harmonic and anharmonic coherent acoustic dynamics in layered Ge-111/Si-111 and bulk GaAs-111 samples. Future improvements in high-average power short-pulse lasers will enable the study of a wider class of materials such as amorphous solids or liquid-phase dynamics of simple molecules, while proposed 4th generation light sources based upon single-pass X-ray free-electron lasers will permit singleshot structural determination of complex biomolecules.
We apply ultrafast time‐resolved X‐ray diffraction to directly study coherent acoustic and optical phonons in laser‐excited materials. In Au the ps acoustic response has been investigated with the particular goal to clarify the interplay of electronic and thermal pressure contributions. In Bi the extreme softening of the coherently excited A 1 g optical phonon presents strong indication that upon intense laser‐excitation the Peierls‐transition which determines the equilibrium structure of Bi can be reversed. In FeRh we studied the lattice response after a fast laser‐induced anti‐ferromagnetic to ferromagnetic phase transition.