High-order harmonic generation (HHG) by an atom in an elliptically polarized laser field is studied numerically and theoretically. We derive equations describing the effect of the driving ellipticity on the HHG efficiency, harmonic ellipticity, and rotation angle for the cases of the ground state with the orbital angular momentum $l=0$ and $l\ne 0$. These equations provide good agreement with the results of our three-dimensional time-dependent Schrödinger equation calculations, as well as with the published experimental data. We show that HHG sensitivity to the driving laser ellipticity increases with the drive wavelength. This predicts high efficiency of the polarization gating schemes using midinfrared laser fields. Furthermore, our study shows significant enhancement of the harmonic ellipticity near the Cooper minimum.

We study high-order harmonic generation from a laser-produced tin plasma using 780 and 390 nm, 40 fs, 1 kHz pulses. Varying the chirp of the laser radiation, we observe variation of the harmonic frequency and intensity. The enhanced 16th and 17th harmonics are attributed to the influence of the strong ionic transitions of tin. Theoretical calculations of the photoabsorption spectra reveal the decisive role of Sn ii and Sn iii transitions in the enhancement of single harmonics. Varying the fundamental frequency we study numerically the spectral width where the harmonic is enhanced. We find, both theoretically and experimentally, that this width is wider than the one of the corresponding resonance in the photoabsorption spectrum. The resonance line modification can be explained by the Stark shift of the autoionizing state in the laser field, as well as the photoionization of this state.

The topological response of matter to electromagnetic fields is a highly demanded property in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantiosensitive optical response of chiral molecules could therefore enhance the efficiency and robustness of chiral optical discrimination. Here we achieve such a topological embedding by introducing the concept of chiral topological light—a light beam which displays chirality locally, with an azimuthal distribution of its handedness described globally by a topological charge. The topological charge is mapped onto the azimuthal intensity modulation of the non-linear optical response, where enantiosensitivity is encoded into its spatial rotation. The spatial rotation is robust against intensity fluctuations and imperfect local polarization states of the driving field. Our theoretical results show that chiral topological light enables detection of percentage-level enantiomeric excesses in randomly oriented mixtures of chiral molecules, opening a way to new, extremely sensitive and robust chiro-optical spectroscopies with attosecond time resolution.

We present a high-order harmonic generation theory which generalizes the strong-field approximation to the resonant case when the harmonic frequency is close to that of the transition from the ground state to an autoionizing state of the generating system. We show that the line shape of the resonant harmonic is a product of the Fano-like factor and the harmonic line which would be emitted in the absence of the resonance. The theory predicts rapid variation of the harmonic phase in the vicinity of the resonance. The calculated resonant harmonic phase is in reasonable agreement with recent measurements. Predicting the phase locking of a group of resonantly enhanced harmonics, our theory allows us to study the perspectives of producing an attosecond pulse train using such harmonics.

We have studied high-order harmonic generation (HHG) in an indium ablation plume driven by intense few-cycle laser pulses centered at 775 nm as a function of the frequency chirp of the laser pulse. We found experimentally that resonant emission lines between 19.7 eV and 22.3 eV (close to the 13th and 15th harmonic of the laser) exhibit a strong, asymmetric chirp dependence, with pronounced intensity modulations. The chirp dependence is reproduced by our numerical time-dependent Schrödinger equation simulations of a resonant HHG by the model indium ion. As demonstrated with our separate simulations of HHG within the strong field approximation, the resonance can be understood in terms of the chirp-dependent HHG photon energy coinciding with the energy of an autoionizing state to ground state transition with high oscillator strength. This supports the validity of the general theory of resonant four-step HHG in the few-cycle limit.