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The advancement of contemporary ultrafast science requires reliable sources to provide high-energy few-cycle light pulses. Through experiments and simulations, we demonstrate an arrangement of pulse postcompression, referred to as cascaded focus and compression (CASCADE), for generating millijoule-level, single-cycle pulses in a compact fashion. CASCADE is realized by a series of foci in matter, whereas pulse compression is provided immediately after each focus to maintain a high efficiency of spectral broadening. By implementing four stages of CASCADE in argon cells, we achieve 50-fold compression of millijoule-level pulses at 1030 nanometers from 157 to 3.1 femtoseconds, with an output pulse energy of 0.98 millijoules and a transmission efficiency of 73%. When driving high harmonic generation, these single-cycle pulses enable the creation of a carrier-envelope phase-dependent extreme ultraviolet continuum with energies extending up to 180 electron volts, providing isolated attosecond pulses at the output.

Polarization engineering and characterization of coherent high-frequency radiation are essential to investigate and control the symmetry properties of light–matter interaction phenomena at their most fundamental scales. This work demonstrates that polarization control and characterization of high-harmonic generation provides an excellent ellipsometry tool that can fully retrieve both the amplitude and phase of a strong-field-driven dipole response. The polarization control of high-harmonic generation is realized by a transient nonlinear dipole grating coherently induced by two noncollinear counterrotating laser fields. By adjusting the ellipticity of the two driving pulses simultaneously, the polarization state of every high-harmonic order can be tuned from linear to highly elliptical, and it is fully characterized through an energy-resolved extreme ultraviolet polarimeter. From the analysis of the polarization state, the ellipsometry indicated that both the amplitude and phase of the high-harmonic dipole scale rapidly with the driving laser field for higher-order harmonics, and, especially, for gases with a small ionization potential. Our experimental results were corroborated by theoretical simulations. Our findings revealed a novel high-harmonic ellipsometry technique that can be used for the next generation of high-harmonic spectroscopy and attosecond metrology studies because of its ability to provide single-digit attosecond accuracy. Our work also paves the way to precisely quantify the strong-field dynamics of fundamental processes associated with the transfer of energy and angular momentum between electron/spin systems and the symmetry-dependent properties of molecules and materials.

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