Extreme Ultraviolet High Harmonics Research Articles

In situ high-harmonic microscopy of a nanostructured solid

Nanostructured optical surfaces allow exquisite control over linear and nonlinear light interactions, where the surface actively creates new frequencies up to high-order harmonics of an intense infrared driving laser field. The function and performance of these surfaces depend sensitively on the distribution of the high-harmonic fields in and between the nanostructured elements, as the high-harmonic wavelength becomes comparable to the nanoscale features of the surface. Imaging the nonlinear response at the active surface with nanometer resolution would greatly benefit the optimization of the metasurface's function. Here we demonstrate an approach to lensless imaging of extreme ultraviolet high harmonics that resolves the amplitude and phase of nonlinear polarization at the active nanostructured surface of an MgO crystal. Imaging the near-field distribution of high harmonics is the gateway to optimized functional high-harmonic metasurfaces and the integration of high harmonics on a chip.

Photon counting of extreme ultraviolet high harmonics using a superconducting nanowire single-photon detector

Laser-driven light sources in the extreme ultraviolet range (EUV) enable nanoscopic imaging with unique label-free elemental contrast. However, to fully exploit the unique properties of these new sources, novel detection schemes need to be developed. Here, we show in a proof-of-concept experiment that superconducting nanowire single-photon detectors (SNSPD) can be utilized to enable photon counting of a laser-driven EUV source based on high harmonic generation (HHG). These detectors are dark-count free and accommodate very high count rates—a perfect match for high repetition rate HHG sources. In addition to the advantages of SNSPDs for classical imaging applications with laser-driven EUV sources, the ability to count single photons paves the way for very promising applications in quantum optics and quantum imaging with high energetic radiation like, e.g., quantum ghost imaging with nanoscale resolution.

Attosecond synchronization of extreme ultraviolet high harmonics from crystals

The interaction of strong near-infrared (NIR) laser pulses with wide-bandgap dielectrics produces high harmonics in the extreme ultraviolet (XUV) wavelength range. These observations have opened up the possibility of attosecond metrology in solids, which would benefit from a precise measurement of the emission times of individual harmonics with respect to the NIR laser field. Here we show that, when high-harmonics are detected from the input surface of a magnesium oxide crystal, a bichromatic probing of the XUV emission shows a clear synchronization largely consistent with a semiclassical model of electron–hole recollisions in bulk solids. On the other hand, the bichromatic spectrogram of harmonics originating from the exit surface of the 200 μm-thick crystal is strongly modified, indicating the influence of laser field distortions during propagation. Our tracking of sub-cycle electron and hole re-collisions at XUV energies is relevant to the development of solid-state sources of attosecond pulses.

Extreme high field plasmonics: Electron acceleration and XUV harmonic generation from ultrashort surface plasmons

Experiments on the excitation of propagating surface plasmons (SPs) by an ultrashort, high intensity laser interaction with grating targets are reviewed. At intensities exceeding 1019 W cm−2 on target, i.e., in the strongly relativistic regime of electron dynamics, multi-megaelectronvolt electrons are accelerated by the SP field as dense bunches collimated in a near-tangent direction. By the use of a suitable blazed grating, the bunch charge can be increased up to ≈660 pC. Intense extreme ultraviolet high harmonics (HHs) diffracted by the grating are observed when a plasma with a submicrometer scale is produced at the target surface by a controlled prepulse. When the SP is excited, the HHs are strongly enhanced in a direction quasi-parallel to the electrons. Simulations suggest that the HHs are boosted by nanobunching in the SP field of the electrons which scatter the laser field. Besides the static and dynamic tailoring of the target density profile, further control of electron and HH emission might be achieved by changing the SP duration using a laser pulse with a rotating wavefront. The latter technique may allow the production of nearly single-cycle SPs.

Probing periodic potential of crystals via strong-field re-scattering

Strong-field ionization and re-scattering phenomena have been used to image angstrom-scale structures of isolated molecules in the gas phase. These methods typically make use of the anisotropic response of the participating molecular orbital. Recently, an anisotropic strong-field response has also been observed in high-order harmonic generation (HHG) from bulk crystals (2016 Nat. Phys. 13 345). In a (100) cut magnesium oxide crystal, extreme ultraviolet high-harmonics are found to depend strongly on the crystal structure and inter-atomic bonding. Here, we extend these measurements to other two important crystal orientations: (111) and (110). We find that HHG from these orientations is also strongly anisotropic. The underlying dynamics is understood using a real-space picture, where high-harmonics are produced via coherent collision of strong-field driven electrons from the atomic sites, including from the nearest neighbor atoms. We find that harmonic efficiency is enhanced when semi-classical electron trajectories connect to the concentrated valence charge distribution regions around the atomic cores. Similarly, the efficiency is suppressed when the trajectories miss the atomic cores. These results further support the real-space picture of HHG with implications for retrieving the periodic potential of the crystal, if not the wavefunctions in three-dimensions.

Laser waveform control of extreme ultraviolet high harmonics from solids.

Solid-state high-harmonic sources offer the possibility of compact, high-repetition-rate attosecond light emitters. However, the time structure of high harmonics must be characterized at the sub-cycle level. We use strong two-cycle laser pulses to directly control the time-dependent nonlinear current in single-crystal MgO, leading to the generation of extreme ultraviolet harmonics. We find that harmonics are delayed with respect to each other, yielding an atto-chirp, the value of which depends on the laser field strength. Our results provide the foundation for attosecond pulse metrology based on solid-state harmonics and a new approach to studying sub-cycle dynamics in solids.

Generation of bright phase-matched circularly-polarized extreme ultraviolet high harmonics

Circularly-polarized extreme UV and X-ray radiation provides valuable access to the structural, electronic and magnetic properties of materials. To date, this capability was available only at large-scale X-ray facilities such as synchrotrons. Here we demonstrate the first bright, phase-matched, extreme UV circularly-polarized high harmonics and use this new light source for magnetic circular dichroism measurements at the M-shell absorption edges of Co. We show that phase matching of circularly-polarized harmonics is unique and robust, producing a photon flux comparable to the linearly polarized high harmonic sources that have been used very successfully for ultrafast element-selective magneto-optic experiments. This work thus represents a critical advance that makes possible element-specific imaging and spectroscopy of multiple elements simultaneously in magnetic and other chiral media with very high spatial and temporal resolution, using tabletop-scale setups.

Time- and angle-resolved photoemission spectroscopy with optimized high-harmonic pulses using frequency-doubled Ti:Sapphire lasers

Time- and angle-resolved photoemission spectroscopy (trARPES) using femtosecond extreme ultraviolet high harmonics has recently emerged as a powerful tool for investigating ultrafast quasiparticle dynamics in correlated-electron materials. However, the full potential of this approach has not yet been achieved because, to date, high harmonics generated by 800nm wavelength Ti:Sapphire lasers required a trade-off between photon flux, energy and time resolution. Photoemission spectroscopy requires a quasi-monochromatic output, but dispersive optical elements that select a single harmonic can significantly reduce the photon flux and time resolution. Here we show that 400nm driven high harmonic extreme-ultraviolet trARPES is superior to using 800nm laser drivers since it eliminates the need for any spectral selection, thereby increasing photon flux and energy resolution to <150meV while preserving excellent time resolution of about 30fs.