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J Itatani

Publications and source records attributed to J Itatani.

4 recordsLinked to original sources

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.

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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.

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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.

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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.

Journal Article↗