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1. Enhancing high-order harmonic generation by controlling the diffusion of the electron wave packet

   https://doi.org/10.1364/OPTICA.422711  

   Severt, T. ; Troß, J. ; Kolliopoulos, G. ; Ben-Itzhak, I. ; Trallero-Herrero, C. A. ( August 2021 , Optica)

   We experimentally study the enhancement of high-order harmonic generation (HHG) driven by synthesized$\mathrm{\omega <\#comment/>}-<\#comment/>3\mathrm{\omega <\#comment/>}$laser fields, where we control whether the ionization rate or the electron wave packet’s diffusion is the dominant enhancement mechanism. When minimizing the electron wave packet’s diffusion, the excursion times of the corresponding electron trajectories are reduced by a factor of 2 or more. This result is important for imaging techniques that use the returning electron wave packet to probe the remaining ion. Furthermore, we achieve a$10\times <\#comment/>$to$3800\times <\#comment/>$enhancement of the harmonic yield driven by the bichromatic fields relative to that of an optimized single-color field, showing that the bichromatic fields improve HHG’s capability as a light source. We also measure that the two-color field’s harmonics have half the divergence angle compared to their single-color counterpart, suggesting that the “short” electron trajectories play a more prominent role compared to their “long” trajectory counterparts, thus improving the wavefront of the emerging harmonic beam.

    

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2. Ultrafast 1  MHz vacuum-ultraviolet source via highly cascaded harmonic generation in negative-curvature hollow-core fibers

   https://doi.org/10.1364/OPTICA.395688  

   Couch, David E. ; Hickstein, Daniel D. ; Winters, David G. ; Backus, Sterling J. ; Kirchner, Matthew S. ; Domingue, Scott R. ; Ramirez, Jessica J. ; Durfee, Charles G. ; Murnane, Margaret M. ; Kapteyn, Henry C. ( July 2020 , Optica)

   Vacuum-ultraviolet (VUV) light is critical for the study of molecules and materials, but the generation of femtosecond pulses in the VUV region at high repetition rates has proven difficult. Here we demonstrate the efficient generation of VUV light at megahertz repetition rates using highly cascaded four-wave mixing processes in a negative-curvature hollow-core fiber. Both even- and odd-order harmonics are generated up to the 15th harmonic (69 nm, 18.0 eV), with high energy resolution of$\sim <\#comment/>40\mathrm{m}\mathrm{e}\mathrm{V}$. In contrast to direct high harmonic generation, this highly cascaded harmonic generation process requires lower peak intensity and therefore can operate at higher repetition rates, driven by a robust$\sim <\#comment/>10\mathrm{W}$fiber-laser system in a compact setup. Additionally, we present numerical simulations that explore the fundamental capabilities and spatiotemporal dynamics of highly cascaded harmonic generation. This VUV source can enhance the capabilities of spectroscopies of molecular and quantum materials, such as photoionization mass spectrometry and time-, angle-, and spin-resolved photoemission.

    

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3. Single-pulse, reference-free, spatiospectral measurement of ultrashort pulse-beams

   https://doi.org/10.1364/OPTICA.462586  

   Goldberger, David ; Barolak, Jonathan ; Bevis, Charles S. ; Ivanic, Bojana ; Schmidt, David ; Lei, Yuhao ; Kazansky, Peter ; Mancini, Giulia F. ; Durfee, Charles G. ; Adams, Daniel E. ( August 2022 , Optica)

   High-intensity pulse-beams are ubiquitous in scientific investigations and industrial applications ranging from the generation of secondary radiation sources (e.g., high harmonic generation, electrons) to material processing (e.g., micromachining, laser-eye surgery). Crucially, pulse-beams can only be controlled to the degree to which they are characterized, necessitating sophisticated measurement techniques. We present a reference-free, full-field, single-shot spatiospectral measurement technique called broadband single-shot ptychography (BBSSP). BBSSP provides the complex wavefront for each spectral and polarization component in an ultrafast pulse-beam and should be applicable across the electromagnetic spectrum. BBSSP will dramatically improve the application and mitigation of spatiospectral pulse-beam structure.

    

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4. Efficient second-harmonic generation in high Q-factor asymmetric lithium niobate metasurfaces

   https://doi.org/10.1364/OL.413764  

   Kang, Lei ; Bao, Huaguang ; Werner, Douglas H. ( January 2021 , Optics Letters)

   Lithium niobate (LN) has been widely used for second-harmonic generation (SHG) from bulk crystals. Recent studies have reported improved SHG efficiency in LN micro-ring resonators and hybrid waveguiding structures, as well as in LN nanostructures supporting anapole modes and plasmon-assisted dipole resonances. Here we numerically demonstrate that high$Q$-factor resonances associated with symmetry-protected bound states in the continuum can lead to highly efficient frequency doubling in LN metasurfaces. Simulations show that the radiative$Q$-factor and on-resonance field enhancement factor observed in the metasurface are closely dependent on the asymmetric parameter$\mathrm{\alpha <\#comment/>}$of the system. Furthermore, high$Q$-factor resonances boost the SH conversion process in the LN nanostructures. In particular, for a LN metasurface with a$Q$-factor of$\sim <\#comment/>8\times <\#comment/>{10}^4$, a 0.49% peak SH conversion efficiency is achieved at a pump intensity of$3.3{\mathrm{k}\mathrm{W}/\mathrm{c}\mathrm{m}}^2$. This suggests that such high$Q$-factor LN metasurfaces may be good candidates for practical blue–ultraviolet light sources. Our work provides insight into the possible implementation of metadevices based on nanoengineering of conventional nonlinear crystals.

    

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5. Macroscopic properties of high-order harmonic generation from molecular ions

   https://doi.org/10.1364/OL.388758  

   Joyce, T. ; Jaron-Becker, A. ( March 2020 , Optics Letters)

   High harmonic spectroscopy utilizes the extremely nonlinear optical process of high-order harmonic generation (HHG) to measure complex attosecond-scale dynamics within the emitting atom or molecule subject to a strong laser field. However, it can be difficult to compare theory and experiment, since the dynamics under investigation are often very sensitive to the laser intensity, which inevitably varies over the Gaussian profile of a typical laser beam. This discrepancy would usually be resolved by so-called macroscopic HHG simulations, but such methods almost always use a simplified model of the internal dynamics of the molecule, which is not necessarily applicable for high harmonic spectroscopy. In this Letter, we extend the existing framework of macroscopic HHG so that high-accuracyab initiocalculations can be used as the microscopic input. This new (to the best of our knowledge) approach is applied to a recent theoretical prediction involving the HHG spectra of open-shell molecules undergoing nonadiabatic dynamics. We demonstrate that the predicted features in the HHG spectrum unambiguously survive macroscopic response calculations, and furthermore they exhibit a nontrivial angular pattern in the far field.

    

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