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Laser-dressed photoelectron spectroscopy, employing extreme-ultraviolet attosecond pulses obtained by femtosecond-laser-driven high-order harmonic generation, grants access to atomic-scale electron dynamics. Limited by space charge effects determining the admissible number of photoelectrons ejected during each laser pulse, multidimensional (i.e. spatially or angle-resolved) attosecond photoelectron spectroscopy of solids and nanostructures requires high-photon-energy, broadband high harmonic sources operating at high repetition rates. Here, we present a high-conversion-efficiency, 18.4-MHz-repetition-rate cavity-enhanced high harmonic source emitting 5 × 105 photons per pulse in the 25-to-60-eV range, releasing 1 × 1010 photoelectrons per second from a 10-µm-diameter spot on tungsten, at space charge distortions of only a few tens of meV. Broadband, time-of-flight photoelectron detection with nearly 100% temporal duty cycle evidences a count rate improvement between two and three orders of magnitude over state-of-the-art attosecond photoelectron spectroscopy experiments under identical space charge conditions. The measurement time reduction and the photon energy scalability render this technology viable for next-generation, high-repetition-rate, multidimensional attosecond metrology.

We combine high-finesse optical resonators and spatial-spectral interferometry to a highly phase-sensitive investigation technique for nonlinear light-matter interactions. We experimentally validate an ab initio model for the nonlinear response of a resonator housing a gas target, permitting the global optimization of intracavity conversion processes like high-order harmonic generation. We predict the feasibility of driving intracavity high-order harmonic generation far beyond intensity limitations observed in state-of-the-art systems by exploiting the intracavity nonlinearity to compress the pulses in time.

We theoretically and experimentally investigate high-harmonic generation in a 78-MHz enhancement cavity with a transverse mode having on-axis intensity maxima at the focus and minima at an opening in the following mirror. We find that the conversion efficiency is comparable to that achievable with a Gaussian mode, whereas the output coupling efficiency can be significantly improved over any other demonstrated technique. This approach offers additional power scaling advantages and additional degrees of freedom in shaping the harmonic emission, paving the way to high-power extreme-ultraviolet frequency combs and the generation of multi-MHz repetition-rate-isolated attosecond pulses.

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The generation of extreme-ultraviolet (XUV) isolated attosecond pulses (IAPs) has enabled experimental access to the fastest phenomena in nature observed so far, namely the dynamics of electrons in atoms, molecules and solids. However, nowadays the highest repetition rates at which IAPs can be generated lies in the kHz range. This represents a rather severe restriction for numerous experiments involving the detection of charged particles, where the desired number of generated particles per shot is limited by space charge effects to ideally one. Here, we present a theoretical study on the possibility of efficiently producing IAPs at multi- MHz repetition rates via cavity-enhanced high-harmonic generation (HHG). To this end, we assume parameters of state-of-the-art Yb-based femtosecond laser technology to evaluate several time-gating methods which could generate IAPs in enhancement cavities. We identify polarization gating and a new method, employing non-collinear optical gating in a tailored transverse cavity mode, as suitable candidates and analyze these via extensive numerical modeling. The latter, which we dub transverse mode gating (TMG) promises the highest efficiency and robustness. Assuming 0.7 μ J , 5-cycle pulses from the seeding laser and a state-of-the-art enhancement cavity, we show that TMG bares the potential to generate IAPs with photon energies around 100 eV and a photon flux of at least 10 8 photons s − 1 at repetition rates of 10 MHz and higher. This result reveals a roadmap towards a dramatic decrease in measurement time (and, equivalently, an increase in the signal-to-noise ratio) in photoelectron spectroscopy and microscopy. In particular, it paves the way to combining attosecond streaking with photoelectron emission microscopy, affording, for the first time, the spatially and temporally resolved observation of plasmonic fields in nanostructures. Furthermore, it promises the generation of frequency combs with an unprecedented bandwidth for XUV precision spectroscopy.

Isolated attosecond pulses (IAPs) produced through laser-driven high-harmonic generation (HHG) hold promise for unprecedented insight into physical, chemical, and biological processes via attosecond x-ray diffraction and spectroscopy with tabletop sources. Efficient scaling of HHG towards x-ray energies, however, has been hampered by ionization-induced plasma generation impeding the coherent buildup of high-harmonic radiation. Recently, it has been shown that these limitations can be overcome in the socalled "overdriven regime" where ionization loss and plasma dispersion strongly modify the driving laser pulse over small distances, albeit without demonstrating IAPs. Here, we report on experiments contrasting the generation of IAPs at 80 eV in argon with neon via attosecond streaking measurements. Comparing our experimental results to numerical simulations, we conclude that IAPs in argon are generated in the overdriven regime. We introduce a simple expression that fully describes the HHG dipole phase-mismatch contribution, specifically the effect of the blueshift of the driving laser. Furthermore, we present a method to numerically calculate the transient HHG phase mismatch, which allows us to demonstrate the accuracy of the introduced phase-mismatch expression. Finally, we perform simulations for different gases and wavelengths and show that including the full HHG dipole phase-mismatch contribution is important for understanding HHG with long-wavelength, few-cycle laser pulses in high-pressure gas targets, which are currently being employed for scaling isolated attosecond pulse generation beyond extreme ultraviolet (XUV) towards soft-x-ray photon energies.

Modern ultrafast laser architectures enable high-order harmonic generation (HHG) in gases at (multi-) MHz repetition rates, where each atom interacts with multiple pulses before leaving the HHG volume. This raises the question of cumulative plasma effects on the nonlinear conversion. Utilizing a femtosecond enhancement cavity with HHG in argon and on-axis geometric extreme-ultraviolet (XUV) output coupling, we experimentally compare the single-pulse case with a double-pulse HHG regime in which each gas atom is hit by two pulses while traversing the interaction volume. By varying the pulse repetition rate (18.4 and 36.8 MHz) in an 18.4-MHz roundtrip-frequency cavity with a finesse of 187, and leaving all other pulse parameters identical (35-fs, 0.6-μJ input pulses), we observe a dramatic decrease in the overall conversion efficiency (output-coupled power divided by the input power) in the double-pulse regime. The plateau harmonics (25–50 eV) exhibit very similar flux despite the twofold difference in repetition rate and average power. We attribute this to a spatially inhomogeneous plasma distribution that reduces the HHG volume, decreasing the generated XUV flux and/or affecting the spatial XUV beam profile, which reduces the efficiency of output coupling through the pierced mirror. These findings demonstrate the importance of cumulative plasma effects for power scaling of high-repetition-rate HHG in general and for applications in XUV frequency comb spectroscopy and in attosecond metrology in particular.