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We study the phase matching of resonant high-harmonic generation (HHG) and high-order frequency mixing (HFM) in plasma. We solve numerically the propagation equations coupled with the time-dependent Schr\"odinger equation for the nonlinear polarisation. The macroscopic harmonic signal is enhanced in the vicinity of a multiphoton resonance with the transition between the ground and autoionising states of the generating ion. We show that narrow and strong resonances (as for gallium and indium ions) provide compensation of the plasma dispersion in a spectral region above the exact resonance improving the phase matching and leading to a high macroscopic signal. The compensation does not take place for a wider resonance (as for manganese ions), instead the phase matching is achieved in the HFM process. Comparing the XUV generated in manganese plasma and in neon gas, we show that the resonant HHG in plasma is an order of magnitude more effective than in the gas, moreover another order of magnitude can be gained from the propagation using HFM in plasma.

We investigate the production of an isolated attosecond pulse~(IAP) via the phase-matching gating of high-harmonic generation by intense laser pulses. Our study is based on the integration of the propagation equation for the fundamental and generated fields with nonlinear polarisation found via the numerical solution of the time-dependent Schr\"odinger equation. We study the XUV energy as a function of the propagation distance (or the medium density) and find that the onset of the IAP production corresponds to the change from linear to quadratic dependence of this energy on the propagation distance (or density). Finally, we show that the upper limit of the fundamental pulse duration for which the IAP generation is feasible is defined by the temporal spreading of the fundamental pulse during the propagation. This nonlinear spreading is defined by the difference of the group velocities for the neutral and photoionised medium.

The production of brighter coherent XUV radiation by intense laser pulses through the process of high-harmonic generation (HHG) is a central challenge in contemporary nonlinear optics. We study the generation and spatial propagation of high harmonics analytically and via ab initio simulations. We focus on the length scales defining the growth of the harmonic signal with propagation distance and show that the well-known coherence length limits HHG only for relatively low driving intensities. For higher intensities, the photoionisation of the medium, naturally accompanying HHG, leads to essentially transient phase matching and laser frequency blue shift. By systematically taking both of these factors into account, we demonstrate that the behaviour of the harmonic signal at higher intensities is defined by another length scale -- the blue-shift length. In this generation regime the XUV intensity at a given frequency first grows quadratically and then saturates passing the blue-shift length, but the total harmonic efficiency continues growing linearly due to the linear increase of the harmonic line bandwidth. The changeover to this generation regime takes place for all harmonic orders roughly simultaneously. The rate of the efficiency growth is maximal if the static dispersion is compensated by photoelectrons near the centre of the laser pulse. Our theory offers a robust way to choose the generation conditions that optimise the growth of the harmonic signal with propagation.

The topological response of matter to electromagnetic fields is a property in high demand in materials design and metrology due to its robustness against noise and decoherence, stimulating recent advances in ultrafast photonics. Embedding topological properties into the enantio-sensitive 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 enantio-sensitivity 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.

Chiral discrimination, a problem of vital importance, has recently become an emerging frontier in ultrafast physics, with remarkable progress achieved in multiphoton and strong-field regimes. Rydberg excitations, unavoidable in the strong-field regime and intentional for few-photon processes, arise in all these approaches. Here we show how to harness this ubiquitous feature by introducing a new phenomenon, enantiosensitive free-induction decay, steered by a tricolour chiral field at a gentle intensity, structured in space and time. We demonstrate theoretically that an excited chiral molecule accumulates an enantiosensitive phase due to perturbative interactions with the tricolour chiral field, resulting in a spatial phase gradient steering the free-induction decay in opposite directions for opposite enantiomers. Our work introduces a general, extremely sensitive, all-optical, enantiosensitive detection technique which avoids strong fields and takes full advantage of recent advances in structuring light.

The perceived dichotomy between analytical and ab initio approaches to theory in attosecond science is often seen as a source of tension and misconceptions. This Topical Review compiles the discussions held during a round-table panel at the 'Quantum Battles in Attoscience' CECAM virtual workshop, to explore the sources of tension and attempt to dispel them. We survey the main theoretical tools of attoscience -- covering both analytical and numerical methods -- and we examine common misconceptions, including the relationship between ab initio approaches and the broader numerical methods, as well as the role of numerical methods in 'analytical' techniques. We also evaluate the relative advantages and disadvantages of analytical as well as numerical and ab initio methods, together with their role in scientific discovery, told through the case studies of two representative attosecond processes: non-sequential double ionisation and resonant high-harmonic generation. We present the discussion in the form of a dialogue between two hypothetical theoreticians, a numericist and an analytician, who introduce and challenge the broader opinions expressed in the attoscience community., Comment: Proceedings of the round-table panel discussion 'Quantum Battle 3 - Numerical vs Analytical Methods' at the Quantum Battles in Attoscience online conference (https://www.quantumbattles.com/), the livestream for which can be found at https://www.youtube.com/watch?v=VJnFfHVDym4