Title: Breakdown of the single-collision condition for soft x-ray high harmonic generation in noble gases
High harmonic generation (HHG) in atomic gases is generally assumed to originate from photoelectrons that are not perturbed by neighboring particles. In this paper, we study theoretically and experimentally the regime where this approximation breaks down. At high laser intensities, we experimentally find that producing soft x-rays beyond this single-collision condition leads to a strong reduction of the coherent HHG response and appearance of incoherent radiation. We generalize our results to phase-matched HHG with mid-infrared drivers, and determine that aminimum pulse energyis needed to simultaneously phase match the HHG process and keep photoelectrons unperturbed by surrounding particles. Therefore, while previous research showed that HHG efficiency is independent of the driving pulse energy if other experimental parameters are scaled accordingly, we find that this rule no longer applies for high photon energies. Our study thus provides important guidelines for the laser parameters needed for the generation of high flux soft x-ray high harmonics.
AlShafey, Abdallah; Jia, Xu-Yan; Lu, Yuan-Ming; Gong, Shou-Shu; McCaul, Gerard; Bondar, Denys; Randeria, Mohit; Oka, Takashi; Landsman, Alexandra S.(
, Journal of the Optical Society of America B)
The breakdown of a Mott-insulator when subjected to intense laser fields is characterized by the formation of doublon-hole pairs. This breakdown is furthermore evidenced by the production of high harmonics that can be experimentally measured. Here, we present an approach for extracting the doublon-hole correlation length of a Mott insulator. The method is based on a dynamical calculation of the Mott insulator’s rate of charge production in response to an applied strong-field laser pulse. We find that coupling the Mott insulator to a metal drastically increases the correlation length, in support of our recent hypothesis [Phys. Rev. B108,144434(2023)2469-995010.1103/PhysRevB.108.144434] that coupling to a metal enhances the charge fluctuations in the insulator. We confirm our conclusions using density matrix renormalization group (DMRG) calculations. The proposed method can be applied to experimentally measured observables, such as differential reflectivity or the high harmonic generation (HHG) spectrum to extract doublon-hole correlation length.
Abstract We present the results of an experiment investigating the generation of high-order harmonics by a femtosecond near-infrared (NIR) laser pulse in the presence of an extreme ultraviolet (XUV) field provided by a free-electron laser (FEL), a process referred to as XUV-assisted high-order harmonic generation (HHG). Our experimental findings show that the XUV field can lead to a small enhancement in the harmonic yield when the XUV and NIR pulses overlap in time, while a strong decrease of the HHG yield and a red shift of the HHG spectrum is observed when the XUV precedes the NIR pulse. The latter observations are in qualitative agreement with model calculations that consider the effect of a decreased number of neutral emitters but are at odds with the predicted effect of the correspondingly increased ionization fraction on the phase matching. Our study demonstrates the technical feasibility of XUV-assisted HHG experiments at FELs, which may provide new avenues to investigate correlation-driven electron dynamics as well as novel ways to study and control propagation effects and phase matching in HHG.
Rosenzweig, J. B.; Majernik, N.; Robles, R. R.; Andonian, G.; Camacho, O.; Fukasawa, A.; Kogar, A.; Lawler, G.; Miao, Jianwei; Musumeci, P.; et al(
, New Journal of Physics)
Abstract
In the field of beam physics, two frontier topics have taken center stage due to their potential to enable new approaches to discovery in a wide swath of science. These areas are: advanced, high gradient acceleration techniques, and x-ray free electron lasers (XFELs). Further, there is intense interest in the marriage of these two fields, with the goal of producing a very compact XFEL. In this context, recent advances in high gradient radio-frequency cryogenic copper structure research have opened the door to the use of surface electric fields between 250 and 500 MV m−1. Such an approach is foreseen to enable a new generation of photoinjectors with six-dimensional beam brightness beyond the current state-of-the-art by well over an order of magnitude. This advance is an essential ingredient enabling an ultra-compact XFEL (UC-XFEL). In addition, one may accelerate these bright beams to GeV scale in less than 10 m. Such an injector, when combined with inverse free electron laser-based bunching techniques can produce multi-kA beams with unprecedented beam quality, quantified by 50 nm-rad normalized emittances. The emittance, we note, is the effective area in transverse phase space (x,px/mec) or (y,py/mec) occupied by the beam distribution, and it is relevant to achievable beam sizes as well as setting a limit on FEL wavelength. These beams, when injected into innovative, short-period (1–10 mm) undulators uniquely enable UC-XFELs having footprints consistent with university-scale laboratories. We describe the architecture and predicted performance of this novel light source, which promises photon production per pulse of a few percent of existing XFEL sources. We review implementation issues including collective beam effects, compact x-ray optics systems, and other relevant technical challenges. To illustrate the potential of such a light source to fundamentally change the current paradigm of XFELs with their limited access, we examine possible applications in biology, chemistry, materials, atomic physics, industry, and medicine—including the imaging of virus particles—which may profit from this new model of performing XFEL science.
Ultrafast high-brightness X-ray pulses have proven invaluable for a broad range of research. Such pulses are typically generated via synchrotron emission from relativistic electron bunches using large-scale facilities. Recently, significantly more compact X-ray sources based on laser-wakefield accelerated (LWFA) electron beams have been demonstrated. In particular, laser-driven sources, where the radiation is generated by transverse oscillations of electrons within the plasma accelerator structure (so-called betatron oscillations) can generate highly-brilliant ultrashort X-ray pulses using a comparably simple setup. Here, we experimentally demonstrate a method to markedly enhance the parameters of LWFA-driven betatron X-ray emission in a proof-of-principle experiment. We show a significant increase in the number of generated photons by specifically manipulating the amplitude of the betatron oscillations by using our novel Transverse Oscillating Bubble Enhanced Betatron Radiation scheme. We realize this through an orchestrated evolution of the temporal laser pulse shape and the accelerating plasma structure. This leads to controlled off-axis injection of electrons that perform large-amplitude collective transverse betatron oscillations, resulting in increased radiation emission. Our concept holds the promise for a method to optimize the X-ray parameters for specific applications, such as time-resolved investigations with spatial and temporal atomic resolution or advanced high-resolution imaging modalities, and the generation of X-ray beams with even higher peak and average brightness.
Rutledge, Jay; Catanese, Anthony; Hickstein, Daniel D.; Diddams, Scott A.; Allison, Thomas K.; Kowligy, Abijith S.(
, Journal of the Optical Society of America B)
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 the ninth order (333 nm) in chirped periodically poled lithium niobate waveguides driven by phase-stable, 100 fs pulses at 3 µm with 100 MHz repetition rate. A mid-infrared to ultraviolet-visible conversion efficiency as high as 10% is observed, among 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. Accommodating the extreme spectral bandwidth, numerical simulations based on a single broadband envelope equation with only quadratic nonlinearity give estimates for the conversion efficiency within approximately 1 order of magnitude over a wide range of experimental parameters. From this comparison between theory and experiment, 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. We also gain insights into spectral optimization via tuning the waveguide poling profile and pump pulse parameters. These results can inform cascaded HHG in a range of different platforms.
Chevreuil, Pierre-Alexis, Brunner, Fabian, Thumm, Uwe, Keller, Ursula, and Gallmann, Lukas. Breakdown of the single-collision condition for soft x-ray high harmonic generation in noble gases. Optica 9.12 Web. doi:10.1364/OPTICA.471084.
Chevreuil, Pierre-Alexis, Brunner, Fabian, Thumm, Uwe, Keller, Ursula, and Gallmann, Lukas.
"Breakdown of the single-collision condition for soft x-ray high harmonic generation in noble gases". Optica 9 (12). Country unknown/Code not available: Optical Society of America. https://doi.org/10.1364/OPTICA.471084.https://par.nsf.gov/biblio/10386710.
@article{osti_10386710,
place = {Country unknown/Code not available},
title = {Breakdown of the single-collision condition for soft x-ray high harmonic generation in noble gases},
url = {https://par.nsf.gov/biblio/10386710},
DOI = {10.1364/OPTICA.471084},
abstractNote = {High harmonic generation (HHG) in atomic gases is generally assumed to originate from photoelectrons that are not perturbed by neighboring particles. In this paper, we study theoretically and experimentally the regime where this approximation breaks down. At high laser intensities, we experimentally find that producing soft x-rays beyond this single-collision condition leads to a strong reduction of the coherent HHG response and appearance of incoherent radiation. We generalize our results to phase-matched HHG with mid-infrared drivers, and determine that aminimum pulse energyis needed to simultaneously phase match the HHG process and keep photoelectrons unperturbed by surrounding particles. Therefore, while previous research showed that HHG efficiency is independent of the driving pulse energy if other experimental parameters are scaled accordingly, we find that this rule no longer applies for high photon energies. Our study thus provides important guidelines for the laser parameters needed for the generation of high flux soft x-ray high harmonics.},
journal = {Optica},
volume = {9},
number = {12},
publisher = {Optical Society of America},
author = {Chevreuil, Pierre-Alexis and Brunner, Fabian and Thumm, Uwe and Keller, Ursula and Gallmann, Lukas},
}
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