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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. 

Synchronously pumped optical parametric oscillators (OPOs) are highly efficient sources of long-wavelength pulses and nonclassical light, making them invaluable for applications in spectroscopy, metrology, multi-photon microscopy, and quantum computation. Typical systems based on free-space cavities either operate non-degenerately, which limits their efficiency, or use active feedback control to achieve degenerate operation, which limits these systems to dedicated low-noise environments. In this work, we demonstrate a femtosecond monolithically integrated OPO. In contrast with bulk OPOs, our monolithic 10 GHz cavity, based on reverse-proton-exchanged lithium niobate, operates stably without active locking. By detuning the repetition rate of the free-running pump laser from the cavity free spectral range, we control the intracavity pulse dynamics and observe many of the operating regimes previously encountered in free-space degenerate OPOs, such as box-pulsing and quadratic bright-dark solitons (simultons), in addition to non-degenerate operation. When operated in the simulton regime and pumped with 125 fs pulses at 1 µm, this monolithic OPO chip outputs broadband sech²pulses (63 nm, 3 dB) with tens of milliwatts of average power. 

Attosecond photoionization time delays reveal information about the potential energy landscape that an outgoing electron wavepacket probes upon ionization. In this study, we experimentally quantify the dependence of the time delay on the angular momentum of the liberated photoelectrons. For this purpose, we resolved electron quantum-path interference spectra in energy and angle using a two-color attosecond pump–probe photoionization experiment in helium. A fitting procedure of the angle-dependent interference pattern allows us to disentangle the relative phase of all four quantum pathways that are known to contribute to the final photoelectron signal. In particular, we resolve the dependence on angular momentum of the delay of one-photon transitions between continuum states, which is an essential and universal contribution to the total photoionization delay observed in attosecond pump–probe measurements. For such continuum–continuum transitions, we measure a delay between outgoing $s$and $d$electrons as large as 12 attoseconds, close to the ionization threshold in helium. Both single-active-electron and first-principlesab initiosimulations confirm this observation for helium and hydrogen, demonstrating the universality of the observed delays.