Attosecond science promises to reveal the most fundamental electronic dynamics occurring in matter and it can develop further by meeting two linked technological goals related to high-order harmonic sources: improved spectral tunability (allowing selectivity in addressing electronic transitions) and higher photon flux (permitting to measure low cross-section processes). New developments come through parametric waveform synthesis, which provides control over the shape of field transients, enabling the creation of highly-tunable isolated attosecond pulses via high-harmonic generation. Here we demonstrate that the first goal is fulfilled since central energy, spectral bandwidth/shape and temporal duration of isolated attosecond pulses can be controlled by shaping the laser waveform via two key parameters: the relative-phase between two halves of the multi-octave spanning spectrum, and the overall carrier-envelope phase. These results not only promise to expand the experimental possibilities in attosecond science, but also demonstrate coherent strong-field control of free-electron trajectories using tailored optical waveforms.
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http://dx.doi.org/10.1038/s41467-021-26772-0 | DOI Listing |
Nat Commun
January 2025
State Key Laboratory of Precision Spectroscopy, East China Normal University, Shanghai, China.
Partial wave analysis is key to interpretation of the photoionization of atoms and molecules on the attosecond timescale. Here we propose a heterodyne analysis approach, based on the delay-resolved anisotropy parameters to reveal the role played by high-order partial waves during photoionization. This extends the Reconstruction of Attosecond Beating By Interference of Two-photon Transitions technique into the few-photon regime.
View Article and Find Full Text PDFWe 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 PDFiScience
September 2024
Department of Chemistry and Biochemistry, University of California, San Diego, La Jolla, CA 92093, USA.
Quantum coherence governs the outcome and efficiency of photochemical reactions and ultrafast molecular dynamics. Recent ultrafast gas-phase X-ray scattering and electron diffraction have enabled the observation of femtosecond nuclear dynamics driven by vibrational coherence. However, probing attosecond electron dynamics and coupled electron-nuclear dynamics remains challenging.
View Article and Find Full Text PDFWe report on attosecond-scale control of high-harmonic and fast electron emission from plasma mirrors driven by relativistic-intensity near-single-cycle light waves at a kHz repetition rate. By controlling the waveform of the intense light transient, we reproducibly form a sub-cycle temporal intensity gate at the plasma mirror surface, leading to the observation of extreme ultraviolet spectral continua, characteristic of isolated attosecond pulse (IAP) generation. We also observe the correlated emission of a waveform-dependent relativistic electron beam, paving the way toward fully lightwave-controlled dynamics of relativistic plasma mirrors.
View Article and Find Full Text PDFLight Sci Appl
August 2024
IFN-CNR, Piazza Leonardo da Vinci 32, 20133, Milano, Italy.
Isolated attosecond pulse (IAP) generation usually involves the use of short-medium gas cells operated at high pressures. In contrast, long-medium schemes at low pressures are commonly perceived as inherently unsuitable for IAP generation due to the nonlinear phenomena that challenge favourable phase-matching conditions. Here we provide clear experimental evidence on the generation of isolated extreme-ultraviolet attosecond pulses in a semi-infinite gas cell, demonstrating the use of extended-medium geometries for effective production of IAPs.
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