Enhancing and controlling single-atom high-harmonic generation spectra: a time-dependent density-functional scheme

High harmonic generation (HHG) provides a flexible framework for the development of coherent light sources in the extreme-ultraviolet and soft X-ray regimes. However it suffers from low conversion efficiencies as the control of the HHG spectral and temporal characteristics requires manipulating electron trajectories on attosecond time scale. The phase matching mechanism has been employed to selectively enhance specific quantum paths leading to HHG. A few important fundamental questions remain open, among those how much of the enhancement can be achieved by the single-emitter and what is the role of correlations (or the electronic structure) in the selectivity and control of HHG generation. Here we address those questions by examining computationally the possibility of optimizing the HHG spectrum of isolated hydrogen and helium atoms by shaping the slowly varying envelope of a 800 nm, 200-cycles long laser pulse. The spectra are computed with a fully quantum mechanical description, by explicitly computing the time-dependent dipole moment of the systems using a time-dependent density-functional approach (or the single-electron Schrödinger equation for the case of H), on top of a one-dimensional model. The sought optimization corresponds to the selective enhancement of single harmonics, which we find to be significant. This selectivity is entirely due to the single atom response, and not to any propagation or phase-matching effect. Moreover, we see that the electronic correlation plays a role in the determining the degree of optimization that can be obtained

Nonlinear Optics

This chapter provides a brief introduction into the basic nonlinear-optical phenomena and discusses some of the most significant recent advances and breakthroughs in nonlinear optics, as well as novel applications of nonlinear-optical processes and devices. Nonlinear optics is the area of optics that studies the interaction of light with matter in the regime where the response of the material system to the applied electromagnetic field is nonlinear in the amplitude of this field. At low light intensities, typical of non-laser sources, the properties of materials remain independent of the intensity of illumination. The superposition principle holds true in this regime, and light waves can pass through materials or be reflected from boundaries and interfaces without interacting with each other. Laser sources, on the other hand, can provide sufficiently high light intensities to modify the optical properties of materials. Light waves can then interact with each other, exchanging momentum and energy, and the superposition principle is no longer valid. This interaction of light waves can result in the generation of optical fields at new frequencies, including optical harmonics of incident radiation or sum- or difference-frequency signals

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This chapter describes lasers and other sources of coherent light that operate in a wide wavelength range. First, the general principles for the generation of coherent continuous-wave and pulsed radiation are treated including the interaction of radiation with matter, the properties of optical resonators and their modes as well as such processes as Q-switching and mode-locking. The general introduction is followed by sections on numerous types of lasers, the emphasis being on todayʼs most important sources of coherent light, in particular on solid-state lasers and several types of gas lasers. An important part of the chapter is devoted to the generation of coherent radiation by nonlinear processes with optical parametric oscillators, difference- and sum-frequency generation, and high-order harmonics. Radiation in the extended ultraviolet (EUV) and x-ray ranges can be generated by free electron lasers (FEL) and advanced x-ray sources. Ultrahigh light intensities up to 1021 W/cm2 open the door to studies of relativistic laser–matter interaction and laser particle acceleration. The chapter closes with a section on laser stabilization