Wavefront control of subcycle vortex pulses via carrier-envelope-phase tailoring.

The carrier-envelope phase (CEP) of an ultrashort laser pulse is becoming more crucial to specify the temporal characteristic of the pulse's electric field when the pulse duration becomes shorter and attains the subcycle regime; here, the pulse duration of the intensity envelope is shorter than one cycle period of the carrier field oscillation. When this subcycle pulse involves a structured wavefront as is contained in an optical vortex (OV) pulse, the CEP has an impact on not only the temporal but also the spatial characteristics owing to the spatiotemporal coupling in the structured optical pulse. However, the direct observation of the spatial effect of the CEP control has not yet been demonstrated.

Carrier-envelope phase control of synthesized waveforms with two acousto-optic programmable dispersive filters.

We demonstrate the scanning and control of the carrier-envelope phases (CEPs) of two adjacent spectral components totally spanning more than one-octave in the short-wave infrared (SWIR) wavelength region by operating two individual acousto-optic programmable dispersive filters (AOPDFs) applied to each of the two spectral components. The total CEP shift of the synthesized sub-cycle pulse composed of the two spectral components is controlled with simultaneous scans of the two CEPs. The resultant error of the controlled CEP was 642 mrad, so that this technique is useful for searching zero CEP of the synthesized pulse with the maximum field amplitude.

Opening a new route to multiport coherent XUV sources via intracavity high-order harmonic generation.

High-order harmonic generation (HHG) is currently utilized for developing compact table-top radiation sources to provide highly coherent extreme ultraviolet (XUV) and soft X-ray pulses; however, the low repetition rate of fundamental lasers, which is typically in the multi-kHz range, restricts the area of application for such HHG-based radiation sources. Here, we demonstrate a novel method for realizing a MHz-repetition-rate coherent XUV light source by utilizing intracavity HHG in a mode-locked oscillator with an Yb:YAG thin disk laser medium and a 100-m-long ring cavity. We have successfully implemented HHG by introducing two different rare gases into two separate foci and picking up each HH beam.

Optical parametric amplification of sub-cycle shortwave infrared pulses.

Few-cycle short-wave infrared (SWIR) pulses are useful tools for research on strong-field physics and nonlinear optics. Here we demonstrate the amplification of sub-cycle pulses in the SWIR region by using a cascaded BBO-based optical parametric amplifier (OPA) chain. By virtue of the tailored wavelength of the pump pulse of 708 nm, we successfully obtained a gain bandwidth of more than one octave for a BBO crystal.

Sub-10-fs control of dissociation pathways in the hydrogen molecular ion with a few-pulse attosecond pulse train.

The control of the electronic states of a hydrogen molecular ion by photoexcitation is considerably difficult because it requires multiple sub-10 fs light pulses in the extreme ultraviolet (XUV) wavelength region with a sufficiently high intensity. Here, we demonstrate the control of the dissociation pathway originating from the 2pσu electronic state against that originating from the 2pπu electronic state in a hydrogen molecular ion by using a pair of attosecond pulse trains in the XUV wavelength region with a train-envelope duration of ∼4 fs. The switching time from the peak to the valley in the oscillation caused by the vibrational wavepacket motion in the 1sσg ground electronic state is only 8 fs.

Conical third-harmonic generation of optical vortex through ultrashort laser filamentation in air.

We experimentally generate third-harmonic (TH) vortex beams in air by the filamentation of femtosecond pulses produced in a lab-built Ti:sapphire chirped pulse amplifier. The generated TH beam profile is shown to evolve with increasing pump energy. At a sufficiently high pump energy, we observe a conical TH emission of the fundamental vortex and confirm that the conical radiation follows the conservation law for orbital angular momentum.

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

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.

Settling time of a vibrational wavepacket in ionization.

The vibrational wavepacket of a diatomic molecular ion at the time of ionization is usually considered to be generated on the basis of the Franck-Condon principle. According to this principle, the amplitude of each vibrational wavefunction in the wavepacket is given by the overlap integral between each vibrational wavefunction and the ground vibrational wavefunction in the neutral molecule, and hence, the amplitude should be a real number, or equivalently, a complex number the phase of which is equal to zero. Here we report the observation of a non-trivial phase modulation of the amplitudes of vibrational wavefunctions in a wavepacket generated in the ground electronic state of a H₂⁺ molecular ion at the time of ionization.

Frequency-resolved optical gating technique for retrieving the amplitude of a vibrational wavepacket.

We propose a novel method to determine the complex amplitude of each eigenfunction composing a vibrational wavepacket of / molecular ions evolving with a ~10 fs time scale. We find that the two-dimensional spectrogram of the kinetic energy release (KER) of H(+)/D(+) fragments plotted against the time delay of the probe pulse is equivalent to the spectrogram used in the frequency-resolved optical gating (FROG) technique to retrieve the complex amplitude of an ultrashort optical pulse. By adapting the FROG algorithm to the delay-KER spectrogram of the vibrational wavepacket, we have successfully reconstructed the complex amplitude.

Attosecond nonlinear optics using gigawatt-scale isolated attosecond pulses.

High-energy isolated attosecond pulses required for the most intriguing nonlinear attosecond experiments as well as for attosecond-pump/attosecond-probe spectroscopy are still lacking at present. Here we propose and demonstrate a robust generation method of intense isolated attosecond pulses, which enable us to perform a nonlinear attosecond optics experiment. By combining a two-colour field synthesis and an energy-scaling method of high-order harmonic generation, the maximum pulse energy of the isolated attosecond pulse reaches as high as 1.

Resolving vibrational wave-packet dynamics of D2(+) using multicolor probe pulses.

We demonstrate the generation and real-time observation of the vibrational wave packet of D(2)(+) by using a sub-10-fs extreme UV high-harmonic pump pulse and a three-color probe laser pulse whose wavelength ranges from near-IR to vacuum UV. This multicolor pump-probe scheme can provide us with a powerful experimental tool for investigating a variety of wave packets evolving with a time scale of ~20 fs.

Frequency modulation of high-order harmonic fields with synthesis of two-color laser fields.

We report periodical frequency modulation of high-order harmonic fields observed by changing the delay between the driving two-color laser fields consisting of the fundamental and its second harmonic (SH) field. The amplitude of modulation has been up to ∼0.4 eV, which is larger than the bandwidth of the fundamental field.

Infrared two-color multicycle laser field synthesis for generating an intense attosecond pulse.

We propose and demonstrate the generation of a continuum high-order harmonic spectrum by mixing multicycle two-color (TC) laser fields with the aim of obtaining an intense isolated attosecond pulse. By optimizing the wavelength of a supplementary infrared pulse in a TC field, a continuum harmonic spectrum was created around the cutoff region without carrier-envelope phase stabilization. The obtained harmonic spectra clearly show the possibility of generating isolated attosecond pulses from a multicycle TC laser field, which is generated by an 800 nm, 30 fs pulse mixed with a 1300 nm, 40 fs pulse.

Interferometry of attosecond pulse trains in the extreme ultraviolet wavelength region.

The temporal coherence of an attosecond optical field in the extreme ultraviolet wavelength region can be defined in terms of the extent of interference in time domain. We successfully measured this phenomenon both with and without spectral decomposition. We also report the results of using this approach to directly observe both symmetry and symmetry breaking of interference fringes in an attosecond pulse train.

Coherent water window x ray by phase-matched high-order harmonic generation in neutral media.

We demonstrate the generation of a coherent water window x ray by extending the plateau region of high-order harmonics under a neutral-medium condition. The maximum harmonic photon energies attained are 300 and 450 eV in Ne and He, respectively. Our proposed generation scheme, combining a 1.

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+).

Direct amplification of terawatt sub-10-fs pulses in a CPA system of Ti:sapphire laser.

We have developed a chirped pulse amplification system of Ti:sapphire laser generating a 9.9 fs pulse with a pulse energy of 11 mJ at a repetition rate of 10 Hz. Spectral narrowing during amplification is successfully compensated by using specially designed partial mirrors and broadband high-damage-threshold mirrors.

Generation of 0.66-TW pulses at 1 kHz by a Ti:sapphire laser.

A 1-kHz, 0.66-TW Ti:sapphire laser has been developed. We obtained 21-fs, 14-mJ pulses with an extraction efficiency of 32% in the final amplifier.

27-fs extreme ultraviolet pulse generation by high-order harmonics.

Autocorrelation measurement was demonstrated for the first time to our knowledge in the XUV region to measure the width of a high-order harmonic pulse. Two-photon ionization of rare gases was used as a nonlinear process for the autocorrelation measurement. The 27-fs pulse width that was obtained is, to our knowledge, the shortest in the XUV region.

50-W average-power, 480-fs KrF excimer laser with gated gain amplification.

We have developed a 50-W average-power KrF excimer laser with a pulse width of 480 fs by using the method of gated gain amplification at a 200-Hz repetition rate.

Generation of 10- microJ coherent extreme-ultraviolet light by use of high-order harmonics.

We demonstrate the generation of 10-microJ coherent extreme-ultraviolet (XUV) light at wavelengths from 73.6 to 42.6 nm, using high-order harmonics.

Sub-20-fs terawatt-class laser system with a mirrorless regenerative amplifier and an adaptive phase controller.

We have developed an ultrabroadband regenerative amplifier with a mirrorless cavity to eliminate the limitation of bandwidth of dielectric coats on cavity mirrors. The large amount of material dispersion in the Pellin-Broca prisms that are used instead of cavity mirrors is compensated for with a hybrid technique that uses Brewster prism pairs in the regenerative amplifier and an adaptive phase controller of a liquid-crystal spatial light modulator. We obtained a 16-fs pulse width with an energy of 13 mJ, which is to our knowledge the highest energy obtained in the sub-20-fs regime by use of an adaptive phase controller.

157-nm coherent light source as an inspection tool for F(2) laser lithography.

We have developed a 157-nm coherent light source by two-photon resonant four-wave mixing in Xe, with two tunable single-mode 1-kHz Ti:sapphire laser systems at 768 and 681 nm. This light source has been developed to determine the instrumental function of a vacuum ultraviolet spectrometer and to evaluate optical designs for ultra-line-narrowed F(2) laser lithography. The spectral linewidth of the source was less than 0.

Dramatic enhancement of high-order harmonic generation.

We present a dramatic enhancement [Phys. Rev. Lett.

Destructive interference during high harmonic generation in mixed gases.

We report on the first experimental evidence of the destructive and constructive interference of high harmonics generated in a mixed gas of He and Ne, which facilitates the coherent control of high harmonic generation. Theoretically, we develop an analytical model of high harmonic generation in mixed gases and succeed in reproducing the experimental results and deriving the optimization conditions for the process. The observed interference modulation is attributed to the difference between the phases of the intrinsically chirped harmonic pulses from He and Ne, which leads to a novel method for broadband measurement of the harmonic phases and for observing the underlying attosecond electron dynamics.