Sub-two-cycle, carrier-envelope phase-stable, intense optical pulses at 1.6 µm from a BiB3O6 optical parametric chirped-pulse amplifier.

We report on the generation of 9.0 fs, 550 µJ, carrier-envelope phase (CEP)-stabilized optical pulses around 1.6 µm at 1 kHz. Few-cycle IR pulses are obtained from a BiB(3)O(6) optical parametric chirped-pulse amplifier. The amplification of nearly octave-spanning ultrabroad pulses without spectral broadening results in good stability in output energy (0.85% rms) and CEP (160 mrad rms). We observed high harmonics in the water window from a neon cell that corresponds to a laser intensity of 4.1×10(14) W/cm(2).

1.2 mJ sub-4-fs source at 1 kHz from an ionizing gas.

We demonstrate a 1.2 mJ, 3.8 fs, carrier-envelope phase-controlled laser source by novel energy-scalable spectral broadening in an ionizing gas medium, which is widely applicable to sub-10-fs multimillijoule laser systems to obtain sub-2-cycle (<4 fs) multi-millijoule pulses.

Quantum path selection in high-harmonic generation by a phase-locked two-color field.

We report the results of our studies on the selection of the quantum path in high-harmonic generation (HHG) with a relative-phase-locked two-color laser field. It is shown that by tuning the relative phase between fundamental and second-harmonic fields, The timing of tunnel ionization and subsequent electron trajectories on the sub-cycle time scale can be controlled. We have clearly observed a phase-dependent two-step feature in the harmonic spectra that can be attributed to the selection of two major trajectories in the two-color field HHG.

5-fs, Multi-mJ, CEP-locked parametric chirped-pulse amplifier pumped by a 450-nm source at 1 kHz.

We report on the development of an optical parametric chirpedpulse amplifier at a 1-kHz repetition rate with a 5.5-fs pulse duration, a 2.7-mJ pulse energy and carrier-envelope phase-control. The amplifier is pumped by a 450-nm pulse from a frequency-doubled Ti:sapphire laser.

Controlling high harmonic generation with molecular wave packets.

We show that, by controlling the alignment of molecules, we can influence the high harmonic generation process. We observed strong intensity modulation and spectral shaping of high harmonics produced with a rotational wave packet in a low-density gas of N2 or O2. In N2, where the highest occupied molecular orbital (HOMO) has sigma(g) symmetry, the maximum signal occurs when the molecules are aligned along the laser polarization while the minimum occurs when it is perpendicular. In O2, where the HOMO has pi(g) symmetry, the harmonics are enhanced when the molecules are aligned around 45 degrees to the laser polarization. The symmetry of the molecular orbital can be read by harmonics. Molecular wave packets offer a means of shaping attosecond pulses.

Tomographic imaging of molecular orbitals.

Single-electron wavefunctions, or orbitals, are the mathematical constructs used to describe the multi-electron wavefunction of molecules. Because the highest-lying orbitals are responsible for chemical properties, they are of particular interest. To observe these orbitals change as bonds are formed and broken is to observe the essence of chemistry. Yet single orbitals are difficult to observe experimentally, and until now, this has been impossible on the timescale of chemical reactions. Here we demonstrate that the full three-dimensional structure of a single orbital can be imaged by a seemingly unlikely technique, using high harmonics generated from intense femtosecond laser pulses focused on aligned molecules. Applying this approach to a series of molecular alignments, we accomplish a tomographic reconstruction of the highest occupied molecular orbital of N2. The method also allows us to follow the attosecond dynamics of an electron wave packet.

Attosecond spectral shearing interferometry.

We show that the complete characterization of arbitrarily short isolated attosecond x-ray pulses can be achieved by applying spectral shearing interferometry to photoelectron wave packets. These wave packets are coherently produced through the photoionization of atoms by two time-delayed replicas of the x-ray pulse, and are shifted in energy with respect to each other by simultaneously applying a strong laser field. The x-ray pulse is reconstructed with the algorithm developed for optical pulses, which requires no knowledge of ionization physics. Using a 800-nm shearing field, x-ray pulses shorter than approximately 400 asec can be fully characterized.

Attosecond streak camera.

An electron generated by x-ray photoionization can be deflected by a strong laser field. Its energy and angular distribution depends on the phase of the laser field at the time of ionization. This phase dependence can be used to measure the duration and chirp of single sub100-attosecond x-ray pulses.