Parametric amplification of 100 fs mid-infrared pulses in ZnGeP2 driven by a Ho:YAG chirped-pulse amplifier.

We report on the parametric generation of 100 fs sub-6-cycle 40 µJ pulses with the center wavelength at 5.2 µm using a 1 ps 2.1 µm pump laser and a dispersion management scheme based on bulk material. Our optically synchronized amplifier chain consists of a Ho:YAG chirped-pulse amplifier and white-light-seeded optical parametric amplifiers providing simultaneous passive carrier-envelope phase locking of three ultrashort longwave pulses at the pump, signal, and idler wavelengths corresponding, respectively, to 2.1, 3.5, and 5.2 µm. We also demonstrate bandwidth enhancement and efficient control over nonlinear spectral phase in the regime of cascaded χ2 nonlinearity in ZnGeP2.

Broadband mid-infrared pulses from potassium titanyl arsenate/zinc germanium phosphate optical parametric amplifier pumped by Tm, Ho-fiber-seeded Ho:YAG chirped-pulse amplifier.

We present a concept of a white-light-seeded-cascaded mid-infrared (mid-IR) optical parametric amplifier (OPA) based on potassium titanyl arsenate and zinc germanium phosphate nonlinear optical crystals and producing 100-µJ level pulses centered at 5300 nm, with the spectrum supporting four-optical-cycle pulse duration. The OPA is pumped by 2090-nm master oscillator/power amplifier based on a Tm,Ho-fiber laser seeder and a Ho:YAG regenerative amplifier delivering 3.8-mJ sub-ps pulses at a repetition rate of 1 kHz. We validate that output parameters of the OPA are scalable by means of increasing the pulse energy, decreasing the pulse duration and redshifting the central wavelength.

Observation of a shape resonance of the positronium negative ion.

When an electron binds to its anti-matter counterpart, the positron, it forms the exotic atom positronium (Ps). Ps can further bind to another electron to form the positronium negative ion, Ps(-) (e(-)e(+)e(-)). Since its constituents are solely point-like particles with the same mass, this system provides an excellent testing ground for the three-body problem in quantum mechanics. While theoretical works on its energy level and dynamics have been performed extensively, experimental investigations of its characteristics have been hampered by the weak ion yield and short annihilation lifetime. Here we report on the laser spectroscopy study of Ps(-), using a source of efficiently produced ions, generated from the bombardment of slow positrons onto a Na-coated W surface. A strong shape resonance of (1)P(o) symmetry has been observed near the Ps (n=2) formation threshold. The resonance energy and width measured are in good agreement with the result of three-body calculations.

Generation of 5.0 fs, 5.0 mJ pulses at 1kHz using hollow-fiber pulse compression.

We demonstrate methods to increase the energy incident on hollow fibers for spectral broadening by self-phase modulation. We used chirped pulses for spectral broadening, lowering the optical intensity to avoid ionization of the gaseous medium. We also used helium as a nonlinear medium and demonstrated the generation of 5.0fs, 5.0mJ pulses at a repetition rate of 1kHz using a pressure gradient hollow-fiber pulse compressor.

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 1.6 microm laser driver and a neutral Ne gas medium, is efficient and scalable in output yields of the water window x ray. Thus, the precept of the design parameter for a single-shot live-cell imaging by contact microscopy is presented.

Dramatic enhancement of high-order harmonic generation.

We present a dramatic enhancement [Phys. Rev. Lett. 91, 043002 (2003)] of high-order harmonic generation by simultaneous irradiation of booster harmonics. A key feature of our experiment is the use of mixed gases (Xe and He) with different ionization energies. The harmonics from Xe atoms act as a booster to increase the harmonic yield from He by a factor of 4 x 10(3). The dominance of the dramatic enhancement effect is supported by simulation with the time-dependent Schrödinger equation as well as the observed spatial characteristic of the generated harmonics and dependence on medium conditions.

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.

Ellipticity dependence of high-order harmonic generation from aligned molecules.

We report ellipticity dependence of high-order harmonic generation (HHG) from aligned N2, O2, and CO2 molecules. Experimentally, we find that the ellipticity dependence is sensitive to molecular alignment and to the shape and symmetry of the valence orbitals. It is also found that the destructive interference in the recombination process affects the ellipticity dependence. Theoretically, we extend the original Lewenstein model to a more generalized model, which can be applicable to HHG from molecules, by introducing an electron acceleration parameter xi(theta) and by combining the molecular orbital method. The present observations are successfully explained by our model.

Quantum interference during high-order harmonic generation from aligned molecules.

High-order harmonic generation (HHG) from atoms and molecules offers potential application as a coherent ultrashort radiation source in the extreme ultraviolet and soft X-ray regions. In the three-step model of HHG, an electron tunnels out from the atom and may recombine with the parent ion (emitting a high-energy photon) after undergoing laser-driven motion in the continuum. Aligned molecules can be used to study quantum phenomena in HHG associated with molecular symmetries; in particular, simultaneous observations of both ion yields and harmonic signals under the same conditions serve to disentangle the contributions from the ionization and recombination processes. Here we report evidence for quantum interference of electron de Broglie waves in the recombination process of HHG from aligned CO2 molecules. The interference takes place within a single molecule and within one optical cycle. Characteristic modulation patterns of the harmonic signals measured as a function of the pump-probe delay are explained with simple formulae determined by the valence orbital of the molecules. We propose that simultaneous observations of both ion yields and harmonic signals can serve as a new route to probe the instantaneous structure of molecular systems.

Optimal control of multiphoton ionization processes in aligned I2 molecules with time-dependent polarization pulses.

Multiphoton ionization processes in aligned I2 molecules are actively controlled by the homemade pulse shaping system, with which a time-dependent polarization pulse can be generated and controlled. We find a correlation between a femtosecond time-dependent polarization pulse and the production efficiency of evenly or oddly charged molecular ions. We achieve much better controllability of the correlation with a time-dependent polarization pulse than with a pulse having a fixed ellipticity. The results suggest the existence of an unknown tunnel ionization mechanism which is characteristic of a time-dependent polarization pulse. Our experiments point to new directions in optimal control studies with molecular systems, as discussed in the text.