Recent progress in high power ultrafast short-wave and mid-wave infrared lasers has enabled gas-phase high harmonic generation (HHG) in the water window and beyond, as well as the demonstration of HHG in condensed matter. In this Perspective, we discuss the recent advancements and future trends in generating and characterizing soft X-ray pulses from gas-phase HHG and extreme ultraviolet (XUV) pulses from solid-state HHG. Then, we discuss their current and potential usage in time-resolved study of electron and nuclear dynamics in atomic, molecular and condensed matters.

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Attosecond science based on high harmonic generation from gases and solids.

The low-energy, long-lived isomer in 229Th, first studied in the 1970s as an exotic feature in nuclear physics, continues to inspire a multidisciplinary community of physicists. It has stimulated innovative ideas and studies that expand the understanding of atomic and nuclear structure of heavy elements and of the interaction of nuclei with bound electrons and coherent light. Using the nuclear resonance frequency, determined by the strong and electromagnetic interactions inside the nucleus, it is possible to build a highly precise nuclear clock that will be fundamentally different from all other atomic clocks based on resonant frequencies of the electron shell. The nuclear clock will open opportunities for highly sensitive tests of fundamental principles of physics, particularly in searches for violations of Einstein’s equivalence principle and for new particles and interactions beyond the standard model. It has been proposed to use the nuclear clock to search for variations of the electromagnetic and strong coupling constants and for dark matter searches. The 229Th nuclear optical clock still represents a major challenge in view of the tremendous gap of nearly 17 orders of magnitude between the present uncertainty in the nuclear transition frequency (about 0.2 eV, corresponding to ∼48 THz) and the natural linewidth (in the mHz range). Significant experimental progress has been achieved in recent years, which will be briefly reviewed. Moreover, a research strategy will be outlined to consolidate our present knowledge about essential 229mTh properties, to determine the nuclear transition frequency with laser spectroscopic precision, realize different types of nuclear clocks and apply them in precision frequency comparisons with optical atomic clocks to test fundamental physics. Two avenues will be discussed: laser-cooled trapped 229Th ions that allow experiments with complete control on the nucleus–electron interaction and minimal systematic frequency shifts, and Th-doped solids enabling experiments at high particle number and in different electronic environments.

Nuclear clocks for testing fundamental physics

Femtosecond mode-locked lasers producing visible/infrared frequency combs have steadily advanced our understanding of fundamental processes in nature. For example, optical clocks employ frequency-comb techniques for the most precise measurements of time, permitting the search for minuscule drifts of natural constants. Furthermore, the generation of extreme-ultraviolet attosecond bursts synchronized to the electric field of visible/infrared femtosecond pulses affords real-time measurements of electron dynamics in matter. Cavity-enhanced high-order harmonic generation sources uniquely combine broadband vacuum- and extreme-ultraviolet spectral coverage with multimegahertz pulse repetition rates and coherence properties akin to those of frequency combs. Here we review the coming of age of this technology and its recent applications and prospects, including precision frequency-comb spectroscopy of electronic and potentially nuclear transitions, and low-space-charge attosecond-temporal-resolution photoelectron spectroscopy with nearly 100% temporal detection duty cycle. This Review covers the milestones for extreme-ultraviolet frequency combs and their applications. A future impact on the construction of nuclear-based optical clocks and multidimensional attosecond photoelectron spectroscopy of solids is remarked.

Extreme-ultraviolet frequency combs for precision metrology and attosecond science

Temporal dissipative solitons in nonlinear optical resonators are self-compressed, self-stabilizing and indefinitely circulating wave packets. Owing to these properties, they have been harnessed for the generation of ultrashort pulses and frequency combs in active and passive laser architectures, including mode-locked lasers1–4, passive fibre resonators5 and microresonators6–11. Here, we demonstrate the formation of temporal dissipative solitons in a free-space enhancement cavity with a Kerr nonlinearity and a spectrally tailored finesse. By locking a 100-MHz-repetition-rate train of 350-fs, 1,035-nm pulses to this cavity-soliton state, we generate a 37-fs sech²-shaped pulse with a peak-power enhancement of 3,200, which exhibits low-frequency intensity-noise suppression. The power scalability unique to free-space cavities, the unprecedented combination of peak-power enhancement and temporal compression, and the cavity-soliton-specific noise filtering attest to the vast potential of this platform of optical solitons for applications including spatiotemporal filtering and compression of ultrashort pulses and cavity-enhanced nonlinear frequency conversion. Temporal dissipative soliton formation in a free-space femtosecond enhancement cavity with a thin Kerr medium is reported. Locking a 350-fs, 1,035-nm pulse train with a repetition rate of 100 MHz to this cavity-soliton state generates a 37-fs sech2-shaped pulse with a peak-power enhancement of 3,200.

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Temporal solitons in free-space femtosecond enhancement cavities

We generate high-order harmonics at high pulse repetition rates using a turnkey laser. High-order harmonics at 400 kHz are observed when argon is used as target gas. In neon we achieve generation of photons with energies exceeding 90 eV ($\sim$13 nm) at 20 kHz. We measure a photon flux of 4.4$\cdot10^{10}$ photons per second per harmonic in argon at 100 kHz. Many experiments employing high-order harmonics would benefit from higher repetition rates, and the user-friendly operation opens up for applications of coherent extreme ultra-violet pulses in new research areas.

High-order harmonic generation using a high-repetition-rate turnkey laser

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. Space charge effects can distort the results of photoelectron spectroscopic measurements, and usually limit the allowable photon flux in an experiment. Here, the authors present an 18.4 MHz repetition rate high harmonic source in the 25–60 eV range, with a large count rate improvement over state-of-the-art attosecond setups under identical space charge conditions.

High-flux ultrafast extreme-ultraviolet photoemission spectroscopy at 18.4 MHz pulse repetition rate.

We present our current results on the fabrication of arbitrary shaped fiber tapers on our tapering rig using a CO2-laser as heat source. Single mode excitation of multimode fibers as well as changing the fiber geometry in an LPG-like fashion is presented. It is shown that this setup allows for reproducible fabrication of single-mode excitation tapers to extract the fundamental mode (M2 < 1.1) from a 30 μm core having an NA of 0.09.

Fabrication of longitudinally arbitrary shaped fiber tapers

The free-space pupil slicer of Yale University's EXtreme PREcision Spectrograph (EXPRES) at Lowell Observatory's Lowell Discovery Telescope (LDT) is placed in the beam conditioning sub-system of the spectrograph in between fiber feeds for an incoming science fiber at octagonal core dimensions of 66 µm, and a respective outgoing rectangular fiber at half the width and twice the height of the octagonal fiber with core dimensions of 132 x 33 µm2. At this location efficient slicing is accomplished between 380 nm and 680 nm because the near- and far-fields are swapped within a double-scrambler arrangement, thus providing a location to image the pupil. The resolution for EXPRES is ca. 150.000 (the spectrograph design without slicing has a resolution of 75.000), thus the pupil gets sliced two times, and the two images are injected into a rectangular fiber ca. 33x132 µm2 that matches the spectrograph slit at a f-number of 1/4. The pupil slicer provides a throughput of >85%, having only modest losses from reflections on the implemented, precision and miniaturized optics, as well as alignment errors, and the injection of light into the rectangular fiber. We report about the pupil slicer's design, integration and alignment features.

Pupil slicer at high throughput for the EXtreme Precision Spectrograph (EXPRES) at the Lowell Discovery Telescope

A module for spectral combination of five channels with an individual power of 20W each, designed for satellite-based communication, is presented. The channels are selected from the telecommunication ITU grid with a spectral spacing of 400 GHz. The combination is based on volume Bragg gratings, allowing for narrow spacing and combination without loss of near-diffraction-limited beam quality. Thermal effects due to high laser power are investigated. Due to the projected on-board satellite usage, volume and mass as well as vacuum conditions and radiation are considered in the module design. 

O. deVries

Papers

High-flux ultrafast extreme-ultraviolet photoemission spectroscopy at 18.4 MHz pulse repetition rate.

Fabrication of longitudinally arbitrary shaped fiber tapers

Pupil slicer at high throughput for the EXtreme Precision Spectrograph (EXPRES) at the Lowell Discovery Telescope

Towards a space-suitable wavelength-division multiplexer for 5-channel high-power long-range laser communication in the C-and L-band