RESUMEN
Tunable ultrashort pulses in the ultraviolet spectral region are in great demand for a wide range of applications, including spectroscopy and pump-probe experiments. While laser sources capable of producing such pulses exist, they are typically very complex. Notably, resonant dispersive-wave (RDW) emission has emerged as a simple technique for generating such pulses. However, the required pulse energy used to drive the RDW emission, so far, is mostly at the microjoule level, requiring complicated and expensive pump sources. Here, we present our work on lowering the pump energy threshold for generating tuneable deep ultraviolet pulses to the level of tens of nanojoules. We fabricated a record small-core antiresonant fiber with a hollow-core diameter of just 6 µm. When filled with argon, the small mode area enables higher-order soliton propagation and deep ultraviolet (220 to 270 nm) RDW emission from 36 fs pump pulses at 515 nm with the lowest pump energy reported to date (tens of nanojoules). This approach will allow the use of low-cost and compact laser oscillators to drive nonlinear optics in gas-filled fibers for the first time to our knowledge.
RESUMEN
Gas-filled hollow-core fibers 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 fibers 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 fiber 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-fiber systems, especially where the input energy is not constant.
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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 in the supercontinuum formation. When using argon, a supercontinuum extending from 350 nm to 2 µm 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.
RESUMEN
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 with laser pulses 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.
RESUMEN
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 DUV ultrafast laser pulses based on resonant dispersive wave emission in hollow capillary fiber. In a total footprint of only 120cm×75cm, including the ytterbium-based drive laser, we generate pulses between 208nm and 363nm at 50kHz 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-color few-femtosecond DUV pulses.
RESUMEN
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 tunable source from 1030 to â¼700 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 fiber for the first time.
RESUMEN
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 µJ 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.
RESUMEN
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 fiber 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.
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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 27 µJ 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.
RESUMEN
We demonstrate high-energy resonant dispersive-wave emission in the deep ultraviolet (218 to 375 nm) from optical solitons in short (15 to 34 cm) hollow capillary fibers. This down-scaling in length compared to previous results in capillaries is achieved by using small core diameters (100 and 150 µm) and pumping with 6.3 fs pulses at 800 nm. We generate pulses with energies of 4 to 6 µJ across the deep ultraviolet in a 100 µm capillary and up to 11 µJ in a 150 µm 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.
RESUMEN
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 characterize tuneable 3 fs 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.
RESUMEN
A new one-pot procedure that includes an initial titanium-catalyzed intermolecular hydroaminoalkylation of N-allyl-2-bromoanilines with N-methylanilines and a subsequent intramolecular Buchwald-Hartwig amination directly gives access to pharmacologically relevant 1,5-benzodiazepines. The process takes advantage of the excellent regioselectivity of the initial hydroaminoalkylation performed in the presence of a titanium mono(formamidinate) catalyst and the fact that the exclusively formed branched hydroaminoalkylation products can only undergo palladium-catalyzed cyclization to 1,5-benzodiazepines.
RESUMEN
High-order harmonic generation (HHG) arising from the nonperturbative 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 multicycle infrared drivers using hollow capillary fibers (HCFs). Starting from a standard, intense multicycle 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 subcycle 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 multicycle drivers.
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We exploit the phenomenon of resonant dispersive wave (RDW) emission in gas-filled hollow capillary fibres (HCFs) to realize time-resolved photoelectron imaging (TRPEI) measurements with an extremely short temporal resolution. By integrating the output end of an HCF directly into a vacuum chamber assembly we demonstrate two-colour deep ultraviolet (DUV)-infrared instrument response functions of just 10 and 11 fs at central pump wavelengths of 250 and 280 nm, respectively. This result represents an advance in the current state of the art for ultrafast photoelectron spectroscopy. We also present an initial TRPEI measurement investigating the excited-state photochemical dynamics operating in the N-methylpyrrolidine molecule. Given the substantial interest in generating extremely short and highly tuneable DUV pulses for many advanced spectroscopic applications, we anticipate our first demonstration will stimulate wider uptake of the novel RDW-based approach for studying ultrafast photochemistry - particularly given the relatively compact and straightforward nature of the HCF setup.
RESUMEN
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- 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.
RESUMEN
There has been considerable recent interest in tabletop soft X-ray attosecond sources enabled by the new generation of intense, few-cycle laser sources at operating wavelengths longer than 800 nm. In our recent work [Johnson et al., Sci. Adv. 4(5), eaar3761 (2018)], we have demonstrated a new regime for the generation of X-ray attosecond pulses in the water window (284-540 eV) by high-harmonic generation, which resulted in soft X-ray fluxes of ≈109 photons/s and a maximum photon energy of 600 eV, an order of magnitude and 50 eV higher, respectively, than previously attained with few-cycle drivers. Here we present the key elements of our apparatus for the generation and detection of soft X-ray high harmonic radiation in the water window. Of critical importance is a differentially pumped gas target capable of supporting the multi-atmospheric pressures required to phase-match the high energy emission while strongly constraining the gas density, suppressing the effects of ionization and absorption outside the interaction region.
RESUMEN
Laser-driven high-harmonic generation provides the only demonstrated route to generating stable, tabletop attosecond x-ray pulses but has low flux compared to other x-ray technologies. We show that high-harmonic generation can produce higher photon energies and flux by using higher laser intensities than are typical, strongly ionizing the medium and creating plasma that reshapes the driving laser field. We obtain high harmonics capable of supporting attosecond pulses up to photon energies of 600 eV and a photon flux inside the water window (284 to 540 eV) 10 times higher than previous attosecond sources. We demonstrate that operating in this regime is key for attosecond pulse generation in the x-ray range and will become increasingly important as harmonic generation moves to fields that drive even longer wavelengths.
RESUMEN
The interaction of intense laser pulses with nanoscale 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 (103 to 105 atoms) using two-cycle 1.8 µm 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 3 keV is observed using laser pulses with a wavelength of 1.8 µm and an intensity of 1 × 1015 W/cm2, whereas only electrons below 500 eV are observed at 800 nm 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.
RESUMEN
An easily accessible formamidinate ligand-bearing titanium complex initially synthesized by Eisen et al. is used as catalyst for intermolecular hydroaminoalkylation reactions of unactivated, sterically demanding 1,1- and 1,2-disubstituted alkenes and styrenes with secondary amines. The corresponding reactions, which have never been achieved with titanium catalysts before, take place with excellent regioselectivity (up to 99 : 1) and in addition, corresponding reactions of 1,3-butadienes with N-methylbenzylamine are also described for the first time.