High-harmonic generation (HHG) is a nonlinear physical process used for the production of ultrashort pulses in XUV region, which are then used for investigating ultrafast phenomena in time-resolved spectroscopies. Moreover, HHG signal itself encodes information on electronic structure and dynamics of the target, possibly coupled to the nuclear degrees of freedom. Investigating HHG signal leads to HHG spectroscopy, which is applied to atoms, molecules, solids and recently also to liquids. Analysing the number of generated harmonics, their intensity and shape gives a detailed insight of, e.g., ionisation and recombination channels occurring in the strong-field dynamics. A number of valuable theoretical models has been developed over the years to explain and interpret HHG features, with the three-step model being the most known one. Originally, these models neglect the complexity of the propagating electronic wavefunction, by only using an approximated formulation of ground and continuum states. Many effects unravelled by HHG spectroscopy are instead due to electron correlation effects, quantum interference, and Rydberg-state contributions, which are all properly captured by anelectronic-structure approach. In this review we have collected recent advances in modelling HHG by means oftime-dependent approaches relying on the propagation of the time-dependent Schrödinger equation (or derived equations) in presence of a very intense electromagnetic field. We limit ourselves to gas-phase atomic and molecular targets, and to solids. We focus on the various levels of theory employed for describing the electronic structure of the target, coupled with strong-field dynamics and ionisation approaches, and on the basis used to represent electronic states. Selected applications and perspectives for future developments are also given.
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http://dx.doi.org/10.1088/1361-648X/ac3608 | DOI Listing |
Nature
January 2025
Department of Physics and Astronomy, University of California, Los Angeles, Los Angeles, CA, USA.
Microscopy and crystallography are two essential experimental methodologies for advancing modern science. They complement one another, with microscopy typically relying on lenses to image the local structures of samples, and crystallography using diffraction to determine the global atomic structure of crystals. Over the past two decades, computational microscopy, encompassing coherent diffractive imaging (CDI) and ptychography, has advanced rapidly, unifying microscopy and crystallography to overcome their limitations.
View Article and Find Full Text PDFJ Chem Theory Comput
January 2025
State Key Laboratory for Mesoscopic Physics and Collaborative Innovation Center of Quantum Matter, School of Physics, Peking University, Beijing 100871, China.
We report on continuous high-harmonic generation (HHG) at 1 kHz repetition rate from a liquid-sheet plasma mirror driven by relativistic-intensity near-single-cycle light transients. Through precise control of both the surface plasma density gradient and the driving light waveform, we can produce highly stable and reproducible extreme ultraviolet spectral quasi-continua, expected to correspond to the generation of stable kHz-trains of isolated attosecond pulses in the time domain. This confirms the exciting potential of liquid-sheet targets as one of the building blocks of future high-power attosecond lasers.
View Article and Find Full Text PDFJ Chem Theory Comput
December 2024
Max Planck Institute for the Structure and Dynamics of Matter, Luruper Ch 149, Hamburg 22761, Germany.
High-harmonic generation (HHG) is a nonlinear process in which a material sample is irradiated by intense laser pulses, causing the emission of high harmonics of incident light. HHG has historically been explained by theories employing a classical electromagnetic field, successfully capturing its spectral and temporal characteristics. However, recent research indicates that quantum-optical effects naturally exist or can be artificially induced in HHG, such as entanglement between emitted harmonics.
View Article and Find Full Text PDFCommun Phys
December 2024
LaserLaB, Department of Physics and Astronomy, Vrije Universiteit Amsterdam, De Boelelaan 1081, 1081 HV Amsterdam, the Netherlands.
Laser spectroscopy of atomic hydrogen and hydrogen-like atoms is a powerful tool for tests of fundamental physics. The 1-2 transition of hydrogen in particular is a cornerstone for stringent Quantum Electrodynamics (QED) tests and for an accurate determination of the Rydberg constant. We report laser excitation of the 1-2 transition in singly-ionized helium (He), a hydrogen-like ion with much higher sensitivity to QED than hydrogen itself.
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