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Ultrafast laser sources in the far ultraviolet (100 nm to 300 nm) have been the subject of intense experimental efforts for several decades, driven primarily by the requirements of advanced experiments in ultrafast science. Resonant dispersive wave emission from high-energy laser pulses undergoing soliton self-compression in a gas-filled hollow capillary fibre promises to meet several of these requirements for the first time, most importantly by combining wide-ranging wavelength tuneability with the generation of extremely short pulses. In this Perspective, we give an overview of this approach to ultrafast far-ultraviolet sources, including its historical origin and underlying physical mechanism, the state of the art and current challenges, and our view of potential applications both within and beyond ultrafast science., Comment: 16 pages, 5 figures

The nature of the insulator-to-metal phase transition in vanadium dioxide (VO2) is one of the longest-standing problems in condensed-matter physics. Ultrafast spectroscopy has long promised to determine whether the transition is primarily driven by the electronic or structural degree of freedom, but measurements to date have been stymied by their sensitivity to only one of these components and/or their limited temporal resolution. Here we use ultra-broadband few-femtosecond pump-probe spectroscopy to resolve the electronic and structural phase transitions in VO2 at their fundamental time scales. We find that the system transforms into a bad-metallic phase within 10 fs after photoexcitation, but requires another 100 fs to complete the transition, during which we observe electronic oscillations and a partial re-opening of the bandgap, signalling a transient semi-metallic state. Comparisons with tensor-network simulations and density-functional theory calculations show these features originate from oscillations around the equilibrium high-symmetry atomic positions during an unprecedentedly fast structural transition, in which the vanadium dimers separate and untwist with two different timescales. Our results resolve the complete structural and electronic nature of the light-induced phase transition in VO2 and establish ultra-broadband few-femtosecond spectroscopy as a powerful new tool for studying quantum materials out of equilibrium., Comment: 20 pages, 12 figures

High-order harmonic generation (HHG) arising from the non-perturbative interaction of intense light fields with matter constitutes a well-established tabletop source of coherent extreme-ultraviolet and soft X-ray radiation, which is typically emitted as attosecond pulse trains. However, ultrafast applications increasingly demand isolated attosecond pulses (IAPs), which offer great promise for advancing precision control of electron dynamics. Yet, the direct generation of IAPs typically requires the synthesis of near-single-cycle intense driving fields, which is technologically challenging. In this work, we theoretically demonstrate a novel scheme for the straightforward and compact generation of IAPs from multi-cycle infrared drivers using hollow capillary fibers (HCFs). Starting from a standard, intense multi-cycle infrared pulse, a light transient is generated by extreme soliton self-compression in a HCF with decreasing pressure, and is subsequently used to drive HHG in a gas target. Owing to the sub-cycle confinement of the HHG process, high-contrast IAPs are continuously emitted almost independently of the carrier-envelope phase (CEP) of the optimally self-compressed drivers. This results in a CEP-robust scheme which is also stable under macroscopic propagation of the high harmonics in a gas target. Our results open the way to a new generation of integrated all-fiber IAP sources, overcoming the efficiency limitations of usual gating techniques for multi-cycle drivers., Comment: 18 pages, 5 figures

We report the flexible on-target delivery of 800 nm wavelength, 5 GW peak power, 40 fs duration laser pulses through an evacuated and tightly coiled 10 m long hollow-core nested anti-resonant fiber by positively chirping the input pulses to compensate for the anomalous dispersion of the fiber. Near-transform-limited output pulses with high beam quality and a guided peak intensity of 3 PW/cm2 were achieved by suppressing plasma effects in the residual gas by pre-pumping the fiber after evacuation. This appears to cause a long-term removal of molecules from the fiber core. Identifying the fluence at the fiber core-wall interface as the damage origin, we scaled the coupled energy to 2.1 mJ using a short piece of larger-core fiber to obtain 20 GW at the fiber output. This scheme can pave the way towards the integration of anti-resonant fibers in mJ-level nonlinear optical experiments and laser-source development.

We experimentally and numerically investigate flat supercontinuum generation in gas-filled anti-resonant guiding hollow-core photonic crystal fiber. By comparing results obtained with either argon or nitrogen we determine the role of the rotational Raman response on the supercontinuum formation. When using argon, a supercontinuum extending from 350 nm to 2 {\mu}m is generated through modulational instability. Although argon and nitrogen exhibit similar Kerr nonlinearity and dispersion, we find that the energy density of the continuum in the normal dispersion region is significantly lower when using nitrogen. Using numerical simulations, we find that due to the closely spaced rotational lines in nitrogen, gain suppression in the fundamental mode causes part of the pump pulse to be coupled into higher-order modes which reduces the energy transfer to wavelengths shorter than the pump.

We experimentally investigate the nonlinear dynamics of ultrashort laser pulses propagating in gas-filled hollow capillary fibres in different dispersion regimes, which are achieved by tuning the gas pressure. When the pulse propagates in the anomalous dispersion regime we observe soliton dynamics accompanied with soliton-plasma effects, such as self-compression, resonant dispersive-wave emission in the fundamental as well as in higher-order modes, soliton blue-shifting and ionisation-induced pulse splitting. Propagation of the pulse in the vicinity of the zero-dispersion wavelength results in pulse splitting and subsequent cross-phase modulation leading to the generation of an additional frequency-shifted band and a 3-octave broad supercontinuum. In the case of pulses propagating in normal dispersion we observe the generation of a broad and flat supercontinuum. In this regime, the experimental results are less well described by simulations that consider only the propagation dynamics inside the fibre. Free-space simulations of the beam propagation in the bulk gas, before the capillary entrance, suggest that this discrepancy is caused by self-focusing and ionisation altering the pulse spatial and temporal shape, affecting both the coupling efficiency and the subsequent propagation inside the capillary.

We investigate soliton self-compression and photoionization effects in an argon-filled antiresonant hollow-core photonic crystal fiber pumped with a commercial Yb:KGW laser. Before the onset of photoionization, we demonstrate self-compression of our 220~fs pump laser to 13~fs in a single and compact stage. By using the plasma driven soliton self-frequency blueshift, we also demonstrate a tuneable source from 1030 to ~700 nm. We fully characterize the compressed pulses using sum-frequency generation time-domain ptychography, experimentally revealing the full time-frequency plasma-soliton dynamics in hollow-core fibre for the first time.

Gas-filled hollow-core fibres are a flexible platform for the manipulation of ultrafast laser pulses through a variety of nonlinear optical effects. Efficient high-fidelity coupling of the initial pulses is very important for system performance. Here we study the effect of self-focusing in gas-cell windows on the coupling of ultrafast laser pulses into hollow-core fibres using (2+1)-dimensional numerical simulations. As expected, we find that the coupling efficiency is degraded and the duration of the coupled pulses changed when the entrance window is too close to the fibre entrance. The interplay of nonlinear spatio-temporal reshaping and the linear dispersion of the window create different results depending on the window material, pulse duration, and pulse wavelength, with longer-wavelength beams more tolerant of high intensity in the window. While shifting the nominal focus to compensate can restore some of the lost coupling efficiency, it improves the pulse duration only marginally. From our simulations we derive a simple expression for the minimum distance between the window and the HCF entrance facet. Our results have implications for the often space-constrained design of hollow-core-fibre systems, especially where the input energy is not constant., Comment: 12 pages, 6 figures

Deep ultraviolet (DUV) laser pulses with tuneable wavelength and very short duration are a key enabling technology for next-generation technology and ultrafast science. Their generation has been the subject of extensive experimental effort, but no technique demonstrated thus far has been able to meet all requirements in one light source. Here we demonstrate a bright, efficient, and compact source of tuneable deep ultraviolet ultrafast laser pulses based on resonant dispersive wave emission in hollow capillary fibre. In a total footprint of only 120 x 75 cm, including the ytterbium-based drive laser, we generate pulses between 208 nm and 363 nm at 50 kHz repetition rate with a total efficiency of up to 3.6%. Down-scaling of the DUV generation reduces the required energy sufficiently to enable the generation of two-colour few-femtosecond DUV pulses., Comment: 5 pages, 5 figures

We investigate soliton self-compression and ultraviolet resonant dispersive wave emission in the higher-order modes of a gas-filled hollow capillary fibre. Our simple analytical scaling rules predict shorter required waveguides and different energy scales when moving from the fundamental to higher-order modes. Experimentally, we demonstrate soliton self-compression and ultraviolet dispersive wave emission in the double-lobe LP$_{11}$ mode of an argon-filled hollow capillary fibre, which we excite by coupling into the fibre at oblique incidence. We observe the generation of ultraviolet dispersive waves which are frequency-shifted and more narrowband as compared to fundamental-mode generation due to the stronger modal dispersion, and a suppression of the supercontinuum between the dispersive wave and the pump pulse. With numerical simulations, we confirm the predictions of our scaling rules and find that the use of higher-order modes can suppress photoionisation and plasma effects even while allowing for much higher pulse energy to be used in the self-compression process. Our results add another degree of freedom for the design of hollow-waveguide systems to generate sub-cycle field transients and tuneable ultrashort laser pulses., Comment: 17 pages, 7 figures

We experimentally demonstrate the efficient generation of circularly polarized pulses tunable from the vacuum to deep ultraviolet (160-380 nm) through resonant dispersive wave emission from optical solitons in a gas-filled hollow capillary fiber. In the deep ultraviolet we measure up to 13 microjoule of pulse energy, and from numerical simulations, we estimate the shortest output pulse duration to be 8.5 fs. We also experimentally verify that simply scaling the pulse energy by 3/2 between linearly and circularly polarized pumping closely reproduces the soliton and dispersive wave dynamics. Based on previous results with linearly polarized self-compression and resonant dispersive wave emission, we expect our technique to be extended to produce circularly polarized few-fs pulses further into the vacuum ultraviolet, and few to sub-fs circularly polarized pulses in the near-infrared.

We numerically investigate the energy and arrival-time noise of ultrashort laser pulses produced via resonant dispersive wave emission in gas-filled hollow-core waveguides under the influence of pump-laser instability. We find that for low pump energy, fluctuations in the pump energy are strongly amplified. However, when the generation process is saturated, the energy of the resonant dispersive wave can be significantly less noisy than that of the pump pulse. This holds for a variety of generation conditions and while still producing few-femtosecond pulses. We further find that the arrival-time jitter of the generated pulse remains well below one femtosecond even for a conservative estimate of the pump pulse energy noise, and that photoionisation and plasma dynamics can lead to exceptional stability for some generation conditions. By applying our analysis to a scaled-down system, we demonstrate that our results hold for frequency conversion schemes based on both small-core microstructured fibre and large-core hollow capillary fibre., Comment: 23 pages, 8 figures

We demonstrate a route to supercontinuum generation in gas-filled hollow-core anti-resonant fibers through the creation of a broad vibrational Raman frequency comb followed by continuous broadening and merging of the comb lines through either rotational Raman scattering or the optical Kerr effect. Our demonstration experiments, utilizing a single pump pulse with 20 ps duration at 532 nm in a nitrogen-filled fiber, produce a supercontinuum spanning from 440 nm to 1200 nm, with an additional deep ultraviolet continuum from 250 nm to 360 nm. Numerical results suggest that this approach can produce even broader supercontinuum spectra extending from the ultraviolet to mid-infrared.

Tuneable ultrafast laser pulses are a powerful tool for measuring difficult-to-access degrees of freedom in materials science. In general these experiments require the ability to address resonances and excitations both above and below the bandgap of materials, and to probe their response at the timescale of the fastest non-trivial internal dynamics. This drives the need for ultrafast sources capable of delivering 10-15 fs duration pulses tuneable across the entire visible (VIS) and near infrared (NIR) range, 500 nm - 3000 nm, as well as the characterization of these sources. Here we present a single frequency-resolved optical gating (FROG) system capable of self-referenced characterization of pulses with 10 fs duration across the entire VIS-NIR spectral range. Our system does not require auxiliary beams and only minor reconfiguration for different wavelengths. We demonstrate the system with measurements of pulses across the entire tuning range.

We demonstrate an efficient scheme for the generation of broadband, high-energy, circularly polarized femtosecond laser pulses in the deep ultraviolet through seeded degenerate four-wave mixing in stretched gas-filled hollow capillary fibers. Pumping and seeding with circularly polarized 35 fs pulses centered at 400 nm and 800 nm, respectively, we generate idler pulses centered at 266 nm with more than 25 microjoule of energy and over 95% spectrally averaged ellipticity. Even higher idler energies and broad spectra (27 nm bandwidth) can be obtained at the cost of reduced ellipticity. Our system can be scaled in average power and used in different spectral regions, including the vacuum ultraviolet.

Resonant dispersive wave (RDW) emission in gas-filled hollow waveguides is a powerful technique for the generation of bright few-femtosecond laser pulses from the vacuum ultraviolet to the near infrared. Here we investigate deep-ultraviolet RDW emission in a hollow capillary fibre filled with a longitudinal gas pressure gradient. We obtain broadly similar emission to the constant-pressure case by applying a surprisingly simple scaling rule for the gas pressure and study the energy-dependent dispersive-wave spectrum in detail using simulations. We further find that in addition to enabling dispersion-free delivery to experimental targets, a decreasing gradient also reduces the pulse stretching within the waveguide itself, and that transform-limited pulses with 3 fs duration can be generated by using short waveguides. Our results illuminate the fundamental dynamics underlying this frequency conversion technique and will aid in fully exploiting it for applications in ultrafast science and beyond., Comment: 4 pages, 5 figures

Infrared femtosecond laser pulses are important tools both in strong-field physics, driving X-ray high-harmonic generation, and as the basis for widely tuneable, if inefficient, ultrafast sources in the visible and ultraviolet. Although anomalous material dispersion simplifies compression to few-cycle pulses, attosecond pulses in the infrared have remained out of reach. We demonstrate soliton self-compression of 1800 nm laser pulses in hollow capillary fibers to sub-cycle envelope duration (2 fs) with 27 GW peak power, corresponding to attosecond field transients. In the same system, we generate wavelength-tuneable few-femtosecond pulses from the ultraviolet (300 nm) to the infrared (740 nm) with energy up to 25 $\mu$J and efficiency up to 12 %, and experimentally characterize the generation dynamics in the time-frequency domain. A compact second stage generates multi-$\mu$J pulses from 210 nm to 700 nm using less than 200 $\mu$J of input energy. Our results significantly expand the toolkit available to ultrafast science., Comment: 8 pages, 5 figures

We demonstrate high-energy resonant dispersive-wave emission in the deep ultraviolet (218 to 375 nm) from optical solitons in short (15 to 34cm) hollow capillary fibres. This down-scaling in length compared to previous results in capillaries is achieved by using small core diameters (100 and 150 $\mu$m) and pumping with 6.3 fs pulses at 800 nm. We generate pulses with energies of 4 to 6 $\mu$J across the deep ultraviolet in a 100 $\mu$m capillary and up to 11 $\mu$J in a 150 $\mu$m capillary. From comparisons to simulations we estimate the ultraviolet pulse to be 2 to 2.5 fs in duration. We also numerically study the influence of pump duration on the bandwidth of the dispersive wave., Comment: 5 pages, 3 figures

Optical soliton dynamics can cause the extreme alteration of the temporal and spectral shape of a propagating light pulse. They occur at up to kilowatt peak powers in glass-core optical fibres and the gigawatt level in gas-filled microstructured hollow-core fibres. Here we demonstrate optical soliton dynamics in large-core hollow capillary fibres. This enables scaling of soliton effects by several orders of magnitude to the multi-mJ energy and terawatt peak power level. We experimentally demonstrate two key soliton effects. First, we observe self-compression to sub-cycle pulses and infer the creation of sub-femtosecond field waveforms - a route to high-power optical attosecond pulse generation. Second, we efficiently generate continuously tunable high-energy (1 to 16 $\mu$J) pulses in the vacuum and deep ultraviolet (110 nm to 400 nm) through resonant dispersive-wave emission.These results promise to be the foundation of a new generation of table-top light sources for ultrafast strong-field physics and advanced spectroscopy.

Dispersive wave emission (DWE) in gas-filled hollow-core dielectric waveguides is a promising source of tuneable coherent and broadband radiation, but so far the generation of few-femtosecond pulses using this technique has not been demonstrated. Using in-vacuum frequency-resolved optical gating, we directly characterise tuneable 3fs pulses in the deep ultraviolet generated via DWE. Through numerical simulations, we identify that the use of a pressure gradient in the waveguide is critical for the generation of short pulses., Comment: 5 pages, 4 figures

The interaction of intense laser pulses with nano-scale particles leads to the production of high-energy electrons, ions, neutral atoms, neutrons and photons. Up to now, investigations have focused on near-infrared to X-ray laser pulses consisting of many optical cycles. Here we study strong-field ionization of rare-gas clusters ($10^3$ to $10^5$ atoms) using two-cycle 1.8~$\mu$m laser pulses to access a new interaction regime in the limit where the electron dynamics are dominated by the laser field and the cluster atoms do not have time to move significantly. The emission of fast electrons with kinetic energies exceeding 3keV is observed using laser pulses with a wavelength of 1.8~$\mu$m and an intensity of $1\times 10^{15}$~W/cm$^2$, whereas only electrons below 500eV are observed at 800nm using a similar intensity and pulse duration. Fast electrons are preferentially emitted along the laser polarization direction, showing that they are driven out from the cluster by the laser field. In addition to direct electron emission, an electron rescattering plateau is observed. Scaling to even longer wavelengths is expected to result in a highly directional current of energetic electrons on a few-femtosecond timescale., Comment: Scientific Reports, accepted