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We demonstrate the visualization of ultrafast hydrogen migration in deuterated acetylene dication (C2D2{2+}) by employing the pump-probe Coulomb explosion imaging with sub-10-fs intense laser pulses (9 fs, 0.13 PW/cm{2}, 800 nm). It is shown, from the temporal evolution of the momenta of the fragment ions produced by the three-body explosion, C2D2{3+}-->D{+} + C{+} + CD{+}, that the migration proceeds in a recurrent manner: the deuterium atom first shifts from one carbon site to the other in a short time scale (approximately 90 fs) and then migrates back to the original carbon site by 280 fs, in competition with the molecular dissociation.

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The concept, design and performance of Japan's compact free-electron laser (FEL) facilities, the SPring-8 Compact SASE Source test accelerator (SCSS) and SPring-8 Angstrom Compact free electron LAser (SACLA), and their applications in mainly atomic, molecular and optical science are reviewed. At SCSS, intense, ultrafast FEL pulses at extreme ultraviolet (EUV) wavelengths have been utilized for investigating various multi-photon processes in atoms, molecules and clusters by means of ion and electron spectroscopy. The quantum optical effect superfluorescence has been observed with EUV excitation. A pump–probe technique combining FEL pulses with near infrared laser pulses has been realized to study the ultrafast dynamics of atoms, molecules and clusters in the sub-picosecond regime. At SACLA, deep inner-shell multi-photon ionization by intense x-ray FEL pulses has been investigated. The development of seeded FEL sources for producing transversely and temporally coherent light, as well as the expected impact on advanced science are discussed.

Since the discovery of roaming as an alternative molecular dissociation pathway in formaldehyde (H2CO), it has been indirectly observed in numerous molecules. The phenomenon describes a frustrated dissociation with fragments roaming at relatively large interatomic distances rather than following conventional transition-state dissociation; incipient radicals from the parent molecule self-react to form molecular products. Roaming has been identified spectroscopically through static product channel–resolved measurements, but not in real-time observations of the roaming fragment itself. Using time-resolved Coulomb explosion imaging (CEI), we directly imaged individual “roamers” on ultrafast time scales in the prototypical formaldehyde dissociation reaction. Using high-level first-principles simulations of all critical experimental steps, distinctive roaming signatures were identified. These were rendered observable by extracting rare stochastic events out of an overwhelming background using the highly sensitive CEI method.

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