Femtosecond Optical Laser System with Spatiotemporal Stabilization for Pump-Probe Experiments at SACLA

We constructed a synchronized femtosecond optical laser system with spatiotemporal stabilization for pump-probe experiments at SPring-8 Angstrom Compact Free Electron Laser (SACLA). Stabilization of output power and pointing has been achieved with a small fluctuation level of a few percent by controlling conditions of temperature and air-flow in the optical paths. A feedback system using a balanced optical-microwave phase detector (BOMPD) has been successfully realized to reduce jitter down to 50 fs. We demonstrated the temporal stability with a time-resolved X-ray diffraction measurement and observed the coherent phonon oscillation of the photo-excited Bi without the post-processing using the timing monitor.

Electron-phonon coupling induced intrinsic Floquet electronic structure

Floquet states are a topic of intense contemporary interest, which is often induced by coherent external oscillating perturbation (e.g., laser, or microwave) which breaks the continuous time translational symmetry of the systems. Usually, electron–phonon coupling modifies the electronic structure of a crystal as a non-coherent perturbation and seems difficult to form Floquet states. Surprisingly, we found that the thermal equilibrium electron–phonon coupling in M(MoS)3 and M(MoSe)3 (where M is a metallic element) exhibits a coherent behavior, and the electronic structure can be described by the Floquet theorem. Such a coherent Floquet state is caused by a selective giant electron–phonon coupling, with thermodynamic phonon oscillation serving as a driving force on the electronic part of the system. The quasi-1D Dirac cone at the Fermi energy has its band gap open and close regularly. Similarly, the electric current will oscillate even under a constant voltage.

Ultrafast disordering of vanadium dimers in photoexcited VO2

Many ultrafast solid phase transitions are treated as chemical reactions that transform the structures between two different unit cells along a reaction coordinate, but this neglects the role of disorder. Although ultrafast diffraction provides insights into atomic dynamics during such transformations, diffraction alone probes an averaged unit cell and is less sensitive to randomness in the transition pathway. Using total scattering of femtosecond x-ray pulses, we show that atomic disordering in photoexcited vanadium dioxide (VO2) is central to the transition mechanism and that, after photoexcitation, the system explores a large volume of phase space on a time scale comparable to that of a single phonon oscillation. These results overturn the current understanding of an archetypal ultrafast phase transition and provide new microscopic insights into rapid evolution toward equilibrium in photoexcited matter.

Growth mechanism of 3D graphene-carbon nanotube hybrid structure

In this paper, a novel molecular dynamic model is presented to describe the growth mechanism of three-dimensional (3D) graphene-carbon nanotube (G-CNT) hybrid structure synthesized by catalytic chemical vapor deposition. For this purpose, first, the physisorption of a carbon atom on a graphene sheet (GS) is studied. Then the model is formulated by using kinetic theory and the longitudinal phonon oscillation of adsorbed carbon atoms on GS. Results show that the CNT grows on GS up to 0.3 mm. Also, there is an optimum temperature for growth of the 3D G-CNT hybrid structure, which can be calculated by the presented model. Finally, it is shown that increase of partial pressure leads to increase of length of growing CNT on GS.