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Recent breakthroughs in high repetition-rate extreme ultraviolet (XUV) light sources and photoelectron analyzers have led to dramatic advances in the performance of time-resolved photoemission experiments. In this perspective article, we discuss the application of cavity-enhanced high-order harmonic generation (CE-HHG), with repetition rates exceeding 10 MHz, to photoemission experiments using advanced endstations incorporating time-of-flight photoelectron analyzers. We discuss recent results, perspective on future areas for further technological improvement, and the wide array of science enabled by ultrafast XUV photoemission experiments, now in a qualitatively new regime., Comment: 14 pages, 9 figures

Broadband ultrafast optical spectroscopy methods, such as transient absorption spectroscopy and 2D spectroscopy, are widely used to study molecular dynamics. However, these techniques are typically restricted to optically thick samples, such as solids and liquid solutions. In this article we discuss a cavity-enhanced ultrafast transient absorption spectrometer covering almost the entire visible range with a detection limit of $\Delta$OD $ < 1 \times 10^{-9}$, extending broadband all-optical ultrafast spectroscopy techniques to dilute beams of gas-phase molecules and clusters. We describe the technical innovations behind the spectrometer and present transient absorption data on two archetypical molecular systems for excited-state intramolecular proton transfer, 1'-hydroxy-2'-acetonapthone and salicylideneaniline, under jet-cooled and Ar cluster conditions.

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., Comment: 10 pages, 7 figures

We report on the development of a high-power mid-infrared frequency comb with 100 MHz repetition rate and 100 fs pulse duration. Difference frequency generation is realized between two branches derived from an Er:fiber comb, amplified separately in Yb:fiber and Er:fiber amplifiers. Average powers of 6.7 W and 14.9 W are generated in the 2.9 $\mu$m idler and 1.6 $\mu$m signal, respectively. With high average power, excellent beam quality, and passive carrier-envelope phase stabilization, this light source is a promising platform for generating broadband frequency combs in the far infrared, visible, and deep ultraviolet.

Time- and Angle-resolved photoelectron spectroscopy from surfaces can be used to record the dynamics of electrons and holes in condensed matter on ultrafast time scales. However, ultrafast photoemission experiments using extreme-ultraviolet (XUV) light have previously been limited by either space-charge effects, low photon flux, or limited tuning range. In this article, we describe space-charge-free XUV photoelectron spectroscopy experiments with up to 5 nA of average sample current using a tunable cavity-enhanced high-harmonic source operating at 88 MHz repetition rate. The source delivers $ > 10^{11}$ photons/s in isolated harmonics to the sample over a broad photon energy range from 18 to 37 eV with a spot size of $58 \times 100 \; \mu$m$^2$. From photoelectron spectroscopy data, we place conservative upper limits on the XUV pulse duration and photon energy bandwidth of 93 fs and 65 meV, respectively. The high photocurrent, lack of space charge distortions of the photoelectron spectra, and excellent isolation of individual harmonic orders allow us to observe the laser-assisted photoelectric effect with sideband amplitudes as low as $6 \times 10^{-4}$, enabling time-resolved XUV photoemission experiments in a qualitatively new regime.

Spectroscopy in the molecular fingerprint spectral region (6.5-20 $\mu$m) yields critical information on material structure for physical, chemical and biological sciences. Despite decades of interest and effort, this portion of the electromagnetic spectrum remains challenging to cover with conventional laser technologies. In this report, we present a simple and robust method for generating super-octave, optical frequency combs in the fingerprint region through intra-pulse difference frequency generation in an orientation-patterned gallium phosphide crystal. We demonstrate the utility of this unique coherent light source for high-precision, dual-comb spectroscopy in methanol and ethanol vapor. These results highlight the potential of laser frequency combs for a wide range of molecular sensing applications, from basic molecular spectroscopy to nanoscopic imaging.

We describe methods using frequency combs and optical resonators for recording two-dimensional (2D) ultrafast spectroscopy signals with high sensitivity. By coupling multiple frequency combs to higher-order modes of one or more optical cavities, background-free, cavity-enhanced 2D spectroscopy signals are naturally generated via phase cycling. As in cavity-enhanced ultrafast transient absorption spectroscopy (CE-TAS), the signal to noise is enhanced by a factor proportional to the cavity finesse squared, so even using cavities of modest finesse, a very high sensitivity is expected, enabling ultrafast 2D spectroscopy experiments in dilute molecular beams.

We present a new technique using a frequency comb laser and optical cavities for performing ultrafast transient absorption spectroscopy with improved sensitivity. Resonantly enhancing the probe pulses, we demonstrate a sensitivity of $\Delta$OD $ = 1 \times 10^{-9}/\sqrt{\mbox{Hz}}$ for averaging times as long as 30 s per delay point ($\Delta$OD$_{min} = 2 \times 10^{-10}$). Resonantly enhancing the pump pulses allows us to produce a high excitation fraction at high repetition-rate, so that signals can be recorded from samples with optical densities as low as OD $\approx 10^{-8}$, or column densities $< 10^{10}$ molecules/cm$^2$. This high sensitivity enables new directions for ultrafast spectroscopy.

Extreme ultraviolet frequency combs are a versatile tool with applications including precision measurement, strong-field physics, and solid-state physics. Here we report on an application of extreme ultraviolet frequency combs and their driving lasers for studying strong-field effects in molecular systems. We perform field-free molecular alignment and high-order harmonic generation with aligned molecules in a gas jet at a repetition rate of 154 MHz using a high-powered optical frequency comb inside a femtosecond enhancement cavity. The cavity-enhanced system provides a means to reach suitable intensities to study field-free molecular alignment and enhance the observable effects of the molecule-field interaction. We observe modulations of the driving field, arising from the nature of impulsive stimulated Raman scattering responsible for coherent molecular rotations. We foresee the impact of this work on the study of molecule-based strong-field physics, with improved precision and a more fundamental understanding of the interaction effects on both the field and molecules., Comment: 5 pages, 5 figures

Many atomic and molecular systems of fundamental interest possess resonance frequencies in the extreme ultraviolet (XUV) where laser technology is limited and radiation sources have traditionally lacked long-term phase coherence. Recent breakthroughs in XUV frequency comb technology have demonstrated spectroscopy with unprecedented resolution at the megahertz level, but even higher resolutions are desired for future applications in precision measurement. By characterizing heterodyne beats between two XUV comb sources, we demonstrate the capability for sub-hertz spectral resolution. This corresponds to coherence times >1 s at photon energies up to 20 eV, more than six orders of magnitude longer than previously reported. This work establishes the ability of creating highly phase-stable radiation in the XUV with performance rivaling that of visible light. Furthermore, by direct sampling of the phase of the XUV light originating from high-harmonic generation, we demonstrate precise measurements of attosecond strong-field physics.

Development of the optical frequency comb has revolutionised metrology and precision spectroscopy due to its ability to provide a precise and direct link between microwave and optical frequencies. A novel application of frequency comb technology that leverages both the ultrashort duration of each laser pulse and the exquisite phase coherence of a train of pulses is the generation of frequency combs in the extreme ultraviolet (XUV) via high harmonic generation (HHG) in a femtosecond enhancement cavity. Until now, this method has lacked sufficient average power for applications, which has also hampered efforts to observe phase coherence of the high-repetition rate pulse train produced in the extremely nonlinear HHG process. Hence, the existence of a frequency comb in the XUV has not been confirmed. We have overcome both challenges. Here, we present generation of >200 {\mu}W per harmonic reaching 50 nm, and the observation of single-photon spectroscopy signals for both an argon transition at 82 nm and a neon transition at 63 nm. The absolute frequency of the argon transition has been determined via direct frequency comb spectroscopy. The resolved 10-MHz linewidth of the transition, limited by the transverse temperature of the argon atoms, is unprecedented in this spectral region and places a stringent upper limit on the linewidth of individual comb teeth. Due to the lack of cw lasers, these frequency combs are currently the only promising avenue towards extending ultrahigh precision spectroscopy to below the 100-nm spectral region with a wide range of applications that include spectroscopy of electronic transitions in molecules, experimental tests of bound state and many body quantum electrodynamics in He+ and He, development of next-generation "nuclear" clocks, and searches for spatial and temporal variation of fundamental constants using the enhanced sensitivity of highly charged ions.