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Exploring attosecond science at the angstrom and nanoscale

Final Report Summary - ATTOIM (Exploring attosecond science at the angstrom and nanoscale)

We proposed and demonstrated a new concept of Laser-induced strong-field ionization gas jet tomography.

https://www.nature.com/articles/s41598-017-06814-8

In the framework of this project, we have conceived and have been investigating a novel in-situ method to investigate the high harmonics generating medium itself. Such an in-situ original method is liable to shed light on fundamental aspects of the HHG process,
improve the acuracy of attosecond strong field measurements, and reveal innovative ways to optimize the HHG and attosecond generation processes.

We introduced a novel in-situ strong field ionization tomography approach for characterizing the spatial density distribution of gas jets. We have shown that for typical intensities in high harmonic generation experiments, the strong field ionization mechanism used in our approach provides an improvement in the resolution close to factor of 2 (resolving about 8 times smaller voxel volume), when compared to linear/single-photon imaging modalities. We find, that while the depth of scan in linear tomography is limited by resolution loss due to the divergence of the driving laser beam, in the proposed approach the depth of focus is localized due to the inherent physical nature of strong-field interaction and discuss implications of these findings. We explore key aspects of the proposed method and compare it with commonly used single- and multi-photon imaging mechanisms. The proposed method will be particularly useful for strong field and attosecond science experiments.

A key ingredient in attosecond technology is the generation of attosecond optical pulse trains1 and isolated attosecond pulses2. Currently, the dominant technique for attosecond pulse generation is based on strong field interaction of a driving laser field with gas targets. Typically, an intense femtosecond laser pulse is focused on an atomic or a molecular gas jet. The highly nonlinear electronic response of the medium to the periodic strong driving field, causes high harmonics generation (HHG) of the laser field. In the case of ideal phase-matching, emission from individual atoms or molecules is coherently added in phase, and the total harmonic intensity is therefore proportional to the square of the emitters’ number. However, in reality, there is a delicate interplay between the phases of generated and driving fields that influence the coherent build-up of HHG radiation. Experimentally, this implies, that the efficiency, temporal and spatial profile of the HHG and attosecond pulse generation, depends on both the driving laser spatial and temporal field distribution, as well as on the spatial density distribution of the generating medium itself. Therefore, detailed experimental characterization of the generating medium density distribution is essential for optimization of the attosecond pulse generation process, and the acquisition of a more profound understanding of the underlying physical phenomena.

Tomography is an effective non-destructive technique, which provides 3D image of the internal structure of materials. It is being widely used in medicine, seismology, materials science and many other scientific and industrial areas. Tomographic reconstruction techniques based on linear or perturbative non-linear interaction also have been used to map the spatial density distribution of gas jets. In this paper we present a novel in-situ method, based on strong-field ionization mechanism, to measure the spatial distribution of a generating medium density itself.

In general, theoretical and numerical calculations of the gas space-time density evolution exiting the jet is a highly non-trivial task and is a subject of the active research in the area of computational fluid dynamics (CFD). Our method opens an effective route for experimental validation, and therefore, a means for improving and refining of these gas jet dynamics’ theoretical/computational models.

In summary, we introduced laser induced strong-field tunneling gas jet tomography that features significant resolution improvements when compared with the hitherto used techniques and enables targeted localized measurement in complex environments. We analysed its unique properties and presented a proof of principles experiment. Our method, which is fully compatible with typical HHG and other strong-field experimental set-ups, will allow simple yet robust gas jet density mapping in all those measurements. Attosecond science has long been restricted to spatially averaged measurements that obscure single molecule response to the strong field. Spatial mapping of the generating medium’s density along with measurements of spectrally resolved wavefronts and complete space-time reconstruction of attosecond pulses5 will pave the way to much greater experimental accuracy in attosecond science.
However, the quest for accurate gas jet density characterization goes far beyond attosecond science. Accurate spatial density characterization of gas jets is important for inertial confinement fusion (ICF), x-ray sources, laser particle acceleration (LPA), cold chemistry and other areas of science and engineering. Hitherto only linear tomography modalities were up to the task. Our approach can be easily transferred to all these experiments.