Tomoya Okino

Extreme ultraviolet free electron laser seeded with high-order harmonic of Ti:sapphire laser

The 13th harmonic of a Ti:sapphire (Ti:S) laser in the plateau region was injected as a seeding source to a 250-MeV free-electron-laser (FEL) amplifier. When the amplification conditions were fulfilled, strong enhancement of the radiation intensity by a factor of 650 was observed. The random and uncontrollable spikes, which appeared in the spectra of the Self-Amplified Spontaneous Emission (SASE) based FEL radiation without the seeding source, were found to be suppressed drastically to form to a narrow-band, single peak profile at 61.2 nm. The properties of the seeded FEL radiation were well reproduced by numerical simulations. We discuss the future precept of the seeded FEL scheme to the shorter wavelength region.

Efficient ejection of H3+ from hydrocarbon molecules induced by ultrashort intense laser fields

The ejection processes of hydrogen molecular ion H(3)(+) from 12 kinds of hydrocarbon molecular species, methanol, ethanol, 1-propanol, 2-propanol, acetone, acetaldehyde, methane, ethane, ethylene, allene, 1,3-butadiene, and cyclohexane, induced by intense laser fields (approximately 10(14) W/cm(2)) have been investigated by time-of-flight mass spectroscopy. The observation of the H(3)(+) production with the kinetic energy range of 3.5-5.0 eV from doubly ionized ethylene, allene, 1,3-butadiene, and cyclohexane, which have no methyl groups, showed the existence of the ultrafast hydrogen migration processes that enables three hydrogen atoms to come together to form H(3)(+) within a hydrocarbon molecule.

Two-body Coulomb explosion and hydrogen migration in methanol induced by intense 7 and 21fs laser pulses

Two-body Coulomb explosion with the C-O bond breaking of methanol induced by intense laser pulses with the duration of Delta t=7 and 21 fs is investigated by the coincidence momentum imaging method. When Delta t=7 fs, the angular distribution of recoil vectors of the fragment ions for the direct C-O bond breaking pathway, CH(3)OH(2+)-->CH(3) (+)+OH(+), exhibits a peak deflected from the laser polarization direction by 30 degrees -45 degrees , and the corresponding angular distribution for the migration pathway, CH(2)OH(2) (+)-->CH(2) (+)+H(2)O(+), in which one hydrogen migrates from the carbon site to the oxygen site prior to the C-O bond breaking, exhibits almost the same profile. When the laser pulse duration is stretched to Delta t=21 fs, the angular distributions for the direct and migration pathways exhibit a broad peak along the laser polarization direction probably due to the dynamical alignment and/or the change in the double ionization mechanism; that is, from the nonsequential double ionization to the sequential double ionization. However, the extent of the anisotropy in the migration pathway is smaller than that in the direct pathway, exhibiting a substantial effect of hydrogen atom migration in the dissociative ionization of methanol interacting with the linearly polarized intense laser field.

Communication: Two stages of ultrafast hydrogen migration in methanol driven by intense laser fields

Hydrogen migration in methanol induced by an intense laser field (0.2 PW/cm(2)) is investigated in real time by a pump-probe coincidence momentum imaging method. The observed temporal evolution of the kinetic energy spectra reveals that there are two distinctively different stages in the hydrogen migration processes in the singly charged methanol: ultrafast hydrogen migration occurring within the intense laser field ( approximately 38 fs) and slower postlaser pulse hydrogen migration ( approximately 150 fs).

Tracing ultrafast hydrogen migration in allene in intense laser fields by triple-ion coincidence momentum imaging.

Ultrafast hydrogen migration in allene (CH(2)=C=CH(2)) in intense laser fields was investigated by triple-ion coincidence momentum imaging. The migrating proton covering the entire range of an allene molecule was visualized by the momentum correlation maps and by the geometrical structure of triply charged allene reconstructed from the observed momentum vectors of fragment ions. The extent of hydrogen migration was found to play a decisive role in breaking selectively one of the two initially equivalent C-C chemical bonds that become inequivalent in the course of the hydrogen migration.

Dissociative two-photon ionization of N2 in extreme ultraviolet by intense self-amplified spontaneous emission free electron laser light

Dissociative multiple ionization processes of N2 were investigated by irradiating N2 with an intense extreme ultraviolet (XUV) light at 50.3nm generated by a compact self amplified spontaneous emission free electron laser light source. From the analysis of the momentum distribution of N+ ejected through the Coulomb explosion of N2 and by the single-shot correlation between the yields of N2+ and N+, it was confirmed that double ionization of N2 occurred by the two-photon absorption of the XUV light.

Attosecond nonlinear Fourier transformation spectroscopy of CO2 in extreme ultraviolet wavelength region.

The interferometric autocorrelation functions of attosecond pulse trains in the time domain were measured by detecting CO(2) (2+) as well as the atomic and molecular fragment ions generated via two-photon absorption of intense vacuum ultraviolet-extreme ultraviolet light by CO(2). It was demonstrated that the Fourier transformation of the interferometric autocorrelation functions of the respective fragment ions appearing in a time-of-flight mass spectrum exhibit spectroscopic information in the frequency domain corresponding to the two-photon photofragment excitation spectra of CO(2) and the double ionization excitation spectrum to form CO(2) (2+).

Ejection dynamics of hydrogen molecular ions from methanol in intense laser fields

The ejection of hydrogen molecular ions from two-body Coulomb explosion processes of methanol (CH3OH, CD3OH and CH3OD) in an intense laser field (800 nm, 60 fs, 0.2 PW cm−2) is investigated by a coincidence momentum imaging method. From the coincidence momentum maps, the ejection processes of hydrogen molecular ions, CH3OH2+→ Hm+ + CH(3−m)OH+(m = 2, 3), CD3OH2+→ Dm+ + CH(3−m)OH+(m = 2, 3) and CH3OD2+→ Hm+ + CH(3−m)OD+(m = 2, 3), are identified. Based on the results obtained with isotopically substituted methanol, the isotope effect on the ejection process of hydrogen molecular ions is discussed. Furthermore, the ejection of H/D exchanged hydrogen molecular ions (HD+, HD2+ and H2D+) is identified, and the timescales for the H/D exchanging processes are estimated from the extent of anisotropy in the ejection directions.

Effect of laser parameters on ultrafast hydrogen migration in methanol studied by coincidence momentum imaging.

The effect of intensity, duration, and polarization of ultrashort laser pulses (795 nm, 40-100 fs, and 0.15-1.5 × 10(15) W/cm(2)) on the hydrogen migration in methanol is systematically investigated using Coulomb explosion coincidence momentum imaging. The ratio of the ion yield obtained for the migration pathway CH(3)OH(2+) → CH(2)(+) + OH(2)(+) with respect to the sum of the yields obtained for the migration pathway and for the nonmigration pathway CH(3)OH(2+) → CH(3)(+) + OH(+) exhibits a small (10-20%) but clear dependence on laser pulse properties, that is, the ratio decreases as the laser peak intensity increases but increases when the pulse duration increases as well as when the laser polarization is changed from linear to circular.

Direct observation of an attosecond electron wave packet in a nitrogen molecule.

Attosecond electron wave packet in a molecule is captured by the pump-probe method with a-few-pulse attosecond pulse train. Capturing electron motion in a molecule is the basis of understanding or steering chemical reactions. Nonlinear Fourier transform spectroscopy using an attosecond-pump/attosecond-probe technique is used to observe an attosecond electron wave packet in a nitrogen molecule in real time. The 500-as electronic motion between two bound electronic states in a nitrogen molecule is captured by measuring the fragment ions with the same kinetic energy generated in sequential two-photon dissociative ionization processes. The temporal evolution of electronic coherence originating from various electronic states is visualized via the fragment ions appearing after irradiation of the probe pulse. This observation of an attosecond molecular electron wave packet is a critical step in understanding coupled nuclear and electron motion in polyatomic and biological molecules to explore attochemistry.