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Register a new userGeneration of phase-matched circularly-polarized extreme ultraviolet high harmonics for magnetic circular dichroism spectroscopy
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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.
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Laser-driven high-order harmonic generation (HHG) provides tabletop sources of broadband extreme-ultraviolet (XUV) light with excellent spatial and temporal coherence. These sources are typically operated at low repetition rates, $f_{rep}lesssim$100 kHz, where phase-matched frequency conversion into the XUV is readily achieved. However, there are many applications that demand the improved counting statistics or frequency-comb precision afforded by operation at high repetition rates, $f_{rep}$ > 10 MHz. Unfortunately, at such high $f_{rep}$, phase matching is prevented by the accumulated steady-state plasma in the generation volume, setting stringent limitations on the XUV average power. Here, we use gas mixtures at high temperatures as the generation medium to increase the translational velocity of the gas, thereby reducing the steady-state plasma in the laser focus. This allows phase-matched XUV emission inside a femtosecond enhancement cavity at a repetition rate of 77 MHz, enabling a record generated power of $sim$2 mW in a single harmonic order. This power scaling opens up many demanding applications, including XUV frequency-comb spectroscopy of few-electron atoms and ions for precision tests of fundamental physical laws and constants.
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 $mu$m-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.
We report on the experimental evidence of magnetic helicoidal dichroism, observed in the interaction of an extreme ultraviolet vortex beam carrying orbital angular momentum with a magnetic vortex. Numerical simulations based on classical electromagnetic theory show that this dichroism is based on the interference of light modes with different orbital angular momenta, which are populated after the interaction between the light phase chirality and the magnetic topology. This observation gives insight into the interplay between orbital angular momentum and magnetism, and sets the framework for the development of new analytical tools to investigate ultrafast magnetization dynamics.
High-harmonic generation (HHG) provides short-wavelength light that is useful for precision spectroscopy and probing ultrafast dynamics. We report efficient, phase-coherent harmonic generation up to 9th-order (333 nm) in chirped periodically poled lithium niobate waveguides driven by phase-stable $leq$12-nJ, 100 fs pulses at 3 $mu$m with 100 MHz repetition rate. A mid-infrared to ultraviolet-visible conversion efficiency as high as 10% is observed, amongst an overall 23% conversion of the fundamental to all harmonics. We verify the coherence of the harmonic frequency combs despite the complex highly nonlinear process. Numerical simulations based on a single broadband envelope equation with quadratic nonlinearity give estimates for the conversion efficiency within approximately 1 order of magnitude over a wide range of experimental parameters. From this comparison we identify a dimensionless parameter capturing the competition between three-wave mixing and group-velocity walk-off of the harmonics that governs the cascaded HHG physics. These results can inform cascaded HHG in a range of different platforms.
This work demonstrates nanoscale magnetic imaging using bright circularly polarized high-harmonic radiation. We utilize the magneto-optical contrast of worm-like magnetic domains in a Co/Pd multilayer structure, obtaining quantitative amplitude and phase maps by lensless imaging. A diffraction-limited spatial resolution of 49 nm is achieved with iterative phase reconstruction enhanced by a holographic mask. Harnessing the unique coherence of high harmonics, this approach will facilitate quantitative, element-specific and spatially-resolved studies of ultrafast magnetization dynamics, advancing both fundamental and applied aspects of nanoscale magnetism.
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