Atomic-scale view of the photoinduced structural transition to form sp3-like bonded order phase in graphite.

Photoexcitation of solids often induces structural phase transitions between different ordered phases, some of which are unprecedented and thermodynamically inaccessible. The phenomenon, known as photoinduced structural phase transition (PSPT), is of significant interest to the technological progress of advanced materials processing and the fundamental understanding of material physics. Here, we applied scanning tunnelling microscopy (STM) to directly characterise the primary processes of the PSPT in graphite to form a sp3-like carbon nano-phase called diaphite. The primary challenge was to provide microscopic views of the graphite-to-diaphite transition. On an atomic scale, STM imaging of the photoexcited surface revealed the nucleation and proliferation processes of the diaphite phase; these were governed by the formation of sp3-like interlayer bonds. The growth mode of the diaphite phase depends strongly on the photon energy of excitation laser light. Different dynamical pathways were proposed to explain the formation of a sp3-like interlayer bonding. Potential mechanisms for photon-energy-dependent growth were examined based on the experimental and calculated results. The present results provide insight towards realising optical control of sp2-to-sp3 conversions and the organisation of nanoscale structures in graphene-related materials.

Optical film-thinning of few-layer graphene epitaxially grown on 4H-SiC(0001) surface : Robustness of monolayer-graphene against the photoexcitation.

As the properties of graphene films depend on their stacked atomic layers, their thickness should be accurately controlled to improve their specific properties. However, by existing methods, controlling the homogeneity of graphene films at the atomic level remains difficult. In this work, photo-stimulated structural modifications of few-layer graphene epitaxially grown on 4H-SiC(0001) were studied using Raman scattering spectroscopy and core-level photoemission spectroscopy. Iterative excitation with laser pulses (800nm, 100fs, p-polarized, 250mJ/cm2) changed the graphene-related 2D Raman line, which is composed of three components characterized by their different responses upon photoexcitation: two components decaying at fast and slow rates, and a component highly resistant to excitation. Core-level photoemission spectroscopy revealed that the observed decay of the 2D line was associated with the elimination of carbon atoms from the graphene layers, finally leaving the robust thin film of single-layer graphene by prolonged excitation. Therefore, this work clearly demonstrates the thickness-dependent structural stability of graphene to optical excitation and opens a promising new method for thinning graphene. An underlying mechanism for the photo-stimulated modifications was also proposed.

Imaging energy-, momentum-, and time-resolved distributions of photoinjected hot electrons in GaAs.

Using time-and angle-resolved photoemission spectroscopy, we determine directly energy-, momentum-, and time-resolved distributions of hot electrons photoinjected into the conduction band of GaAs, a prototypical direct-gap semiconductor. The nascent distributions of photoinjected electrons are captured for different pump photon energies and polarization. The evolutions of hot electron distributions in ultrafast intervalley scattering processes are resolved in momentum space with fs-temporal resolution, revealing an intervalley transition time as short as 20 fs.