Highly efficient high-harmonic generation was achieved in helium using a two-color laser field that consisted of the fundamental and the second harmonic fields of a femtosecond Ti:sapphire laser. By applying a high intensity second harmonic, the harmonics generated in the orthogonally polarized twocolor field were stronger than those obtained in the fundamental field by more than 2 orders of magnitude, and even stronger than those of the parallel polarization case. A conversion efficiency as high as 5 10 ÿ5 was obtained for the 38th harmonic at 21.6 nm. The physical origin of this enhancement was deduced by analyzing the electron behavior in the two-color field.

We have achieved very efficient high-harmonic generation in a two-color laser field using a long gas jet of He. With the optimization of laser parameters and target conditions, strong harmonics were produced at 2͑2n +1͒th orders in an orthogonally polarized two-color field. The strongest harmonic at the 38th order ͑21.6 nm͒ reached an energy of 0.6 J with a 6 mm gas jet, giving a conversion efficiency as high as 2 ϫ 10 −4 .

We theoretically investigate the high-order harmonic generation from a neon atom irradiated by an intense two-color femtosecond laser pulse, in which the fundamental field and its second harmonic are linearly polarized and orthogonal to each other. In contrast to usual high-harmonic generation with linearly polarized fundamental field alone, a very strong and clean high-harmonic spectrum, consisting of both odd and even orders of harmonics, can be generated in the orthogonally polarized two-color laser field with proper selection of the relative phase between the fundamental and second-harmonic fields. In time domain, this results in a strong and regular attosecond pulse train. The origin of these behaviors is elucidated by analyzing semiclassical electron paths and by simulating high-harmonic generation quantum mechanically.

Characteristics of high harmonics generated from aligned N 2 molecules were investigated by rotating the molecules with respect to the polarization of harmonic generation pulses. The high harmonics in the plateau and the cutoff regions showed distinctive behaviour, which could be explained from the calculation of transition dipole moments between recolliding electron and multi-orbitals of N 2 molecule consisting of the highest occupied molecular orbital (HOMO) and the lower-lying orbital below HOMO (HOMO-1). It was also observed that the angular dependence of harmonics from aligned molecules with respect to the polarization of harmonic generation pulses was closely related to the geometrical structure of molecular orbitals, and that the harmonic in the transition region from the plateau to the cutoff was influenced comparably by both HOMO and HOMO-1. These results confirmed that high harmonic generation and molecular structure were closely linked.

The spectral structure of harmonics was experimentally controlled by changing the chirp of femtosecond laser pulses, and the dependence of harmonic chirp on atomic species was analysed using harmonics from neon and helium. Experimental results and theoretical analysis based on the Wigner distribution function showed that the spectral structure varied sensitively to laser chirp and the harmonic chirp was determined by the competition between dynamically induced negative chirp and self-phase modulation induced positive chirp. The generation of sharp and bright harmonics was achieved with appropriately chirped laser pulses under given experimental conditions, especially negatively chirped pulses in the case of laser intensity above the saturation intensity for optical-field ionization.

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