Spatiotemporal optical vortex (STOV) pulses carrying purely transverse intrinsic orbital angular momentum (TOAM) are attracting increasing attention because the TOAM provides a new degree of freedom to characterize light–matter interactions. In this paper, using particle-in-cell simulations, we present spatiotemporal high-harmonic generation in the relativistic region, driven by an intense STOV beam impinging on a plasma target. It is shown that the plasma surface acts as a spatial–temporal-coupled relativistic oscillating mirror with various frequencies. The spatiotemporal features are satisfactorily transferred to the harmonics such that the TOAM scales with the harmonic order. Benefitting from the ultrahigh damage threshold of the plasma over the optical media, the intensity of the harmonics can reach the relativistic region. This study provides a new approach for generating intense spatiotemporal extreme ultraviolet vortices and investigating STOV light–matter interactions at relativistic intensities.

We show experimental evidence that, for the intense high-order harmonics from nanoparticles, there is a strong contribution from neutral atoms. We present the results of studies on the harmonics generated in laser-produced plasmas containing various nanoparticles, including Cr2O3, In2O3, Ag, MnTiO3, Sn, Cu, and Au. These results are compared with the harmonics generated from plasma produced on the surface of bulk targets. The harmonic spectrum from nanoparticle and bulk In2O3 show that there is a lack in the resonant enhancement of the 13th harmonic for the former. Along with the relatively low cut-off for nanoparticle harmonics, these results show that it is the neutral atom in the nanoparticle that emits the intense harmonics. Structural studies of plasma debris confirm the presence and integrity of nanoparticles in the plasma plumes.

We describe here the present status of the Advanced Laser Light Source (ALLS) facility, a state-of-the-art multi-beam Ti:sapphire laser system presently under construction in Canada. ALLS is a national user facility to be commissioned in 2005 at the INRS campus near Montreal. The 25 fs ALLS multi-beam laser system has three components, each with different repetition rate and output energy. These multiple laser beams will be used to generate a “rainbow” of femtosecond pulses from the far infrared to hard X-rays, which can be combined to perform unique experiments, such as dynamic molecular imaging. In this paper, we describe two examples of experiments that are planned by our group with the ALLS facility. The first is the highly efficient generation of high-order harmonics using ablation medium. We demonstrate the generation of up to the 53rd harmonics (λ = 15 nm) of a Ti:sapphire laser pulse (150 fs, 10 mJ), using pre-pulse (210 ps, 24 mJ) produced boron ablation as the nonlinear medium. The second example is the demonstration of in-line phase-contrast imaging with an ultrafast (300 fs) laser-based hard X-ray source (Mo K-α line). Images of biological samples have shown great enhancement of contrast due to this technique, distinguishing details that are barely observable or even undetectable in absorption images.

We present a Ramsey technique using high-order harmonics for high-resolution atomic spectroscopy in the extreme ultraviolet. Pairs of time-delayed and phase-coherent harmonic pulses generated by the interaction of ultrashort and intense laser pulses with a noble gas are used to study excited states of krypton.

Strong ionization of the gas medium has significant effects in the process of medium-order harmonic generation. The combined effect of neutral atom depletion and defocusing of the pump beam due to the intensity-dependent density of free electrons, significantly modifies the conversion characteristics and efficiency. For moderate harmonic orders, the yield is optimized for well-defined values of the pump laser intensity that do not depend on the order or on the focusing geometry, but only on the ionization potential of the gas. In particular focusing conditions, the ionization-induced defocusing can effectively guide the pump beam along channels of optimum intensity, thus enhancing the overall conversion efficiency. We demonstrate that a very simple model is able to reproduce all our experimental results in a surprisingly good way.