X-ray crystallography has been central to the development of many fields of science over the past century. It has now matured to a point that as long as good-quality crystals are available, their ...atomic structure can be routinely determined in three dimensions. However, many samples in physics, chemistry, materials science, nanoscience, geology, and biology are noncrystalline, and thus their three-dimensional structures are not accessible by traditional x-ray crystallography. Overcoming this hurdle has required the development of new coherent imaging methods to harness new coherent x-ray light sources. Here we review the revolutionary advances that are transforming x-ray sources and imaging in the 21st century.
We demonstrate, to our knowledge, the first bright circularly polarized high-harmonic beams in the soft X-ray region of the electromagnetic spectrum, and use them to implement X-ray magnetic circular ...dichroism measurements in a tabletop-scale setup. Using counterrotating circularly polarized laser fields at 1.3 and 0.79 μm, we generate circularly polarized harmonics with photon energies exceeding 160 eV. The harmonic spectra emerge as a sequence of closely spaced pairs of left and right circularly polarized peaks, with energies determined by conservation of energy and spin angular momentum. We explain the single-atom and macroscopic physics by identifying the dominant electron quantum trajectories and optimal phase-matching conditions. The first advanced phase-matched propagation simulations for circularly polarized harmonics reveal the influence of the finite phase-matching temporal window on the spectrum, as well as the unique polarization-shaped attosecond pulse train. Finally, we use, to our knowledge, the first tabletop X-ray magnetic circular dichroism measurements at theN4,5
absorption edges of Gd to validate the high degree of circularity, brightness, and stability of this light source. These results demonstrate the feasibility of manipulating the polarization, spectrum, and temporal shape of high harmonics in the soft X-ray region by manipulating the driving laser waveform.
The frequency doubling of laser light was one of the first new phenomena observed following the invention of the laser over 50 years ago. Since then, the quest to extend nonlinear optical ...upconversion to ever-shorter wavelengths has been a grand challenge in laser science. Two decades of research into high-order harmonic generation has recently uncovered several feasible routes for generating bright coherent X-ray beams using small-scale femtosecond lasers. The physics of this technique combines the microscopic attosecond science of atoms driven by intense laser fields with the macroscopic extreme nonlinear optics of phase matching, thus essentially realizing a coherent, tabletop version of the Roentgen X-ray tube.
We generate angularly isolated beams of circularly polarized extreme ultraviolet light through the first implementation of non-collinear high harmonic generation with circularly polarized driving ...lasers. This non-collinear technique offers numerous advantages over previous methods, including the generation of higher photon energies, the separation of the harmonics from the pump beam, the production of both left and right circularly polarized harmonics at the same wavelength and the capability of separating the harmonics without using a spectrometer. To confirm the circular polarization of the beams and to demonstrate the practicality of this new light source, we measure the magnetic circular dichroism of a 20 nm iron film. Furthermore, we explain the mechanisms of non-collinear high harmonic generation using analytical descriptions in both the photon and wave models. Advanced numerical simulations indicate that this non-collinear mixing enables the generation of isolated attosecond pulses with circular polarization.
High-harmonic generation is a universal response of matter to strong femtosecond laser fields, coherently upconverting light to much shorter wavelengths. Optimizing the conversion of laser light into ...soft x-rays typically demands a trade-off between two competing factors. Because of reduced quantum diffusion of the radiating electron wave function, the emission from each species is highest when a short-wavelength ultraviolet driving laser is used. However, phase matching–the constructive addition of x-ray waves from a large number of atoms–favors longer-wavelength mid-infrared lasers. We identified a regime of high-harmonic generation driven by 40-cycle ultraviolet lasers in waveguides that can generate bright beams in the soft x-ray region of the spectrum, up to photon energies of 280 electron volts. Surprisingly, the high ultraviolet refractive indices of both neutral atoms and ions enabled effective phase matching, even in a multiply ionized plasma. We observed harmonics with very narrow linewidths, while calculations show that the x-rays emerge as nearly time-bandwidth-limited pulse trains of ~100 attoseconds.
High-harmonic generation (HHG) traditionally combines ~100 near-infrared laser photons to generate bright, phase-matched, extreme ultraviolet beams when the emission from many atoms adds ...constructively. Here, we show that by guiding a mid-infrared femtosecond laser in a high-pressure gas, ultrahigh harmonics can be generated, up to orders greater than 5000, that emerge as a bright supercontinuum that spans the entire electromagnetic spectrum from the ultraviolet to more than 1.6 kilo-electron volts, allowing, in principle, the generation of pulses as short as 2.5 attoseconds. The multiatmosphere gas pressures required for bright, phase-matched emission also support laser beam self-confinement, further enhancing the x-ray yield. Finally, the x-ray beam exhibits high spatial coherence, even though at high gas density the recolliding electrons responsible for HHG encounter other atoms during the emission process.
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