Extreme-ultraviolet high-order-harmonic pulses with 1.6·10(7) photons/pulse at 32.5 eV have been separated from multiple harmonic orders by a time-preserving monochromator using a single grating in the off-plane mount. This grating geometry gives minimum temporal broadening and high efficiency. The pulse duration of the monochromatized harmonic pulses has been measured to be in the range 20 to 30 fs when the harmonic process is driven by an intense 30 fs near-infrared pulse. The harmonic photon energy is tunable between 12 and 120 eV. The instrument is used in the monochromatized branch of the Artemis beamline at the Central Laser Facility (UK) for applications in ultrafast electron spectroscopy.
The emerging techniques of molecular spectroscopy by high order harmonic generation have hitherto been conducted only with Ti:Sapphire lasers which are restricted to molecules with high ionization potentials. In order to gain information on the molecular structure, a broad enough range of harmonics is required. This implies using high laser intensities which would saturate the ionization of most molecular systems of interest, e.g. organic molecules. Using a laser at 1300 nm, we are able to extend the technique to molecules with relatively low ionization potentials (approximately 11 eV), observing wide harmonic spectra reaching up to 60 eV. This energy range improves spatial resolution of the high harmonic spectroscopy to the point where interference minima in harmonic spectra of N(2)O and C(2)H(2) can be observed.
We demonstrate enhancement by 1 order of magnitude of the high-order harmonics generated in argon by combining a fundamental field at 1300 nm (10(14) W cm(-2)) and its orthogonally polarized second harmonic at 650 nm (2 × 10(13) W cm(-2)) and by controlling the relative phase between them. This extends earlier work by ensuring that the main effect is the combined field steering the electron trajectory with negligible contribution from multiphoton effects compared to the previous schemes with 800/400 nm fields. We access a broad energy range of harmonics (from 20 eV to 80 eV) at a low laser intensity (far below the ionization saturation limit) and observe deep modulation of the harmonic yield with a period of π in the relative phase. Strong field theoretical analysis reveals that this is principally due to the steering of the recolliding electron wave packet by the two-color field. Our modeling also shows that the atto chirp can be controlled, leading to production of shorter pulses.
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