Deep-UV (DUV) supercontinuum (SC) sources based on gas-filled hollow-core fibers constitute perhaps the most viable solution towards ultrafast, compact, and tunable lasers in the UV spectral region. Noise and spectral stability of such broadband sources are key parameters that define their true potential and suitability towards real-world applications. In order to investigate the spectral stability and noise levels in these fiber-based DUV sources, we generate an SC spectrum that extends from 180 nm (through phase-matched dispersive waves - DWs) to 4 μm by pumping an argon-filled hollow-core anti-resonant fiber at a wavelength of 2.45 μm. We characterize the long-term stability of the source over several days and the pulse-to-pulse relative intensity (RIN) noise of the strongest DW at 275 nm. The results indicate no sign of spectral degradation over 110 hours, but the RIN of the DW pulses at 275 nm is found to be as high as 33.3%. Numerical simulations were carried out to investigate the spectral distribution of the RIN and the results confirm the experimental measurements and that the poor noise performance is due to the RIN of the pump laser, which was hitherto not considered in numerical modelling of these sources. The results presented herein provide an important step towards an understanding of the noise mechanism underlying such complex light-gas nonlinear interactions and demonstrate the need for pump laser stabilization.
We present the use of linearly down-tapered gas-filled hollow-core photonic crystal fiber in a single-stage, pumped with pulses from a compact infrared laser source, to generate a supercontinuum carrying significant spectral power in the deep ultraviolet (200 - 300 nm). The generated supercontinuum extends from the near infrared down to around 213 nm with up to 0.83 mW/nm in the deep ultraviolet.
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 produc…
Strong mid-infrared light-matter interaction has attracted extensive attention as it opens up new frontiers in nonlinear optics. Here we observe through simulations a novel aspect of mid-infrared pulse dynamics in a high-pressure gas-filled capillary, where a pulse with a power well below the critical power for Kerr self-focusing undergoes an astonishing rise of the peak intensity following an extremely efficient spectral broadening. This intensity enhancement is attributed to the Kerr-induced focusing of the supercontinuum. Our study provides an interesting perspective for controlling the las…
Nonlinear propagation of intense femtosecond laser pulses in bulk transparent media leads to a specific propagation regime, termed femtosecond filamentation, which in turn produces dramatic spectral broadening, or superbroadening, termed supercontinuum generation. Femtosecond supercontinuum generation in transparent solids represents a compact, efficient and alignment-insensitive technique for generation of coherent broadband radiation at various parts of the optical spectrum, which finds numerous applications in diverse fields of modern ultrafast science. During recent years, this research fi…
In this letter we demonstrate the possibility to determine the temporal and spectral structure (spectrogram) of a complex light pulse exploiting the ultrafast switching character of a non-thermal photo-induced phase transition. As a proof, we use a VO2 multi-film, undergoing an ultrafast insulator-to-metal phase transition when excited by femtosecond near-infrared laser pulses. The abrupt variation of the multi-film optical properties, over a broad infrared/visible frequency range, is exploited to determine, in-situ and in a simple way, the spectrogram of a supercontinuum pulse produced by a p…
We report on the generation of a three-octave-wide supercontinuum extending from the vacuum ultraviolet (VUV) to the near-infrared, spanning at least 113 to 1000 nm (i.e., 11 to 1.2 eV), in He-filled hollow-core kagome-style photonic crystal fiber. Numerical simulations confirm that the main mechanism is a novel and previously undiscovered interaction between dispersive-wave emission and plasma-induced blueshifted soliton recompression around the fiber zero dispersion frequency. The VUV part of the supercontinuum, which modeling shows to be coherent and possess a simple phase structure, has su…
In this Letter, we show theoretically that the nonlinear photoionisation process of a noble gas inside a hollow-core photonic crystal fibre can be exploited in obtaining broadband supercontinuum generation via pumping close to the mid-infrared regime. The interplay between the Kerr and photoionisation nonlinearities is strongly enhanced in this regime. Photoionisation continuously modifies the medium dispersion, in which the refractive index starts to significantly decrease and approach the epsilon-near-zero regime. Subsequently, the self-phase modulation induced by the Kerr effect is boosted …
Although supercontinuum sources are readily available for the visible and near infrared, and recently also for the mid-IR, many areas of biology, chemistry and physics would benefit greatly from the availability of compact, stable and spectrally bright deep ultraviolet (DUV) and vacuum ultraviolet (VUV) supercontinuum sources. Such sources have however not yet been developed. Here we report the generation of a bright supercontinuum, spanning more than three octaves from 124 nm to beyond 1200 nm, in hydrogen-filled kagomé-style hollow-core photonic crystal fiber (kagomé-PCF). Few-μJ, 30 fs pump…
Ultrafast broadband ultraviolet radiation is of importance in spectroscopy and photochemistry, since high photon energies enable single-photon excitations and ultrashort pulses allow time-resolved studies. Here we report the use of gas-filled hollow-core photonic crystal fibers (HC-PCFs) for efficient ultrafast nonlinear optics in the ultraviolet. Soliton self-compression of 400 nm pulses of (unprecedentedly low) ~500 nJ energies down to sub-6-fs durations is achieved, as well as resonant emission of tunable dispersive waves from these solitons. In addition, we discuss the generation of a flat…
Supercontinuum (SC) generation based on ultrashort pulse compression constitutes one of the most promising technologies towards an ultra-wide bandwidth, high-brightness and spatially coherent light sources for applications such as spectroscopy and microscopy. Here, multi-octave SC generation in a gas-filled hollow-core antiresonant fiber (HC-ARF) is reported spanning from 200 nm in the deep ultraviolet (DUV) to 4000 nm in the mid-infrared (mid-IR). A measured average output power of 5 mW was obtained by pumping at the center wavelength of the first anti-resonance transmission window (2460 nm) …
Efficient supercontinuum generation (SCG) requires excitation of solitons at the pump laser wavelength. Quadratic nonlinear waveguides may support an effective self-defocusing nonlinearity so solitons can directly be generated at common ultrafast laser wavelengths without any waveguide dispersion engineering. We here experimentally demonstrate efficient SCG in a standard lithium niobate (LN) waveguide without using quasi-phase matching (QPM). By using femtosecond pumps with wavelengths in the $1.25-1.5 μ\rm m$ range, where LN has normal dispersion and thus supports self-defocusing solitons, oc…
Ultrafast supercontinuum generation in gas-filled waveguides is one enabling technology for many intriguing application ranging from attosecond metrology towards biophotonics, with the amount of spectral broadening crucially depending on the pulse dispersion of the propagating mode. Here we show that the structural resonances in gas-filled anti-resonant hollow core optical fiber provide an additional degree of freedom in dispersion engineering, allowing for the generation of more than three octaves of broadband light ranging deep UV wavelength towards the near infrared.Our observation relies o…
We describe a two-color pump-probe scanning magneto-optical Kerr effect (MOKE) microscope which we have developed to investigate electron spin phenomena in semiconductors at cryogenic temperatures with picosecond time and micrometer spatial resolution. The key innovation of our microscope is the usage of an ultrafast `white light' supercontinuum fiber-laser source which provides access to the whole visible and near-infrared spectral range. Our Kerr microscope allows for the independent selection of the excitation and detection energy while avoiding the necessity to synchronize the pulse trains…
This thesis centres on the development of multidimensional fluorescence imaging tools, with a particular emphasis on fluorescence lifetime imaging (FLIM) microscopy for application to biological research. The key aspects of this thesis are the development and application of tunable supercontinuum excitation sources based on supercontinuum generation in microstructured optical fibres and the development of stimulated emission depletion (STED) microscope capable of fluorescence lifetime imaging beyond the diffraction limit. The utility of FLIM for biological research is illustrated by examples o…
We present a quantitative comparison between the high-pressure fuel spray images obtained experimentally using classical imaging with coherent and incoherent ultrafast illuminations recorded using a compatible CMOS camera. The ultrafast, incoherent illumination source was extracted from the supercontinuum generated by tightly focusing the femtosecond laser pulses in water. The average velocity maps computed using time-correlated image-pairs and spray edge complexity computed using the average curvature scale space maps are compared for the spray images obtained with the two illumination techni…
Gas-filled hollow-core photonic crystal fibre (PCF) is being used to generate ever wider supercontinuum spectra, in particular via dispersive wave (DW) emission in the deep and vacuum ultraviolet, with a multitude of applications. DWs are the result of the resonant transfer of energy from a self-compressed soliton, a process which relies crucially on phase matching. It was recently predicted that, in the strong-field regime, the additional transient anomalous dispersion introduced by gas ionization would allow phase-matched DW generation in the mid-infrared (MIR)-something that is forbidden in…
When an ultrafast optical pulse with high intensity is propagating through transparent material a supercontinuum can be coherently generated by self-phase modulation, which is essential to many photonic applications in fibers and integrated waveguides. However, the presence of dispersion causes stagnation of spectral broadening past a certain propagation length, requiring an increased input peak power for further broadening. We present a concept to drive supercontinuum generation with significantly lower input power by counteracting spectral stagnation via alternating the sign of group velocit…
We demonstrate that time-domain ptychography, a recently introduced ultrafast pulse reconstruction modality, has properties ideally suited for the temporal characterization of complex light pulses with large time-bandwidth products as it achieves temporal resolution on the scale of a single optical cycle using long probe pulses, low sampling rates, and an extremely fast and robust algorithm. In comparison to existing techniques, ptychography minimizes the data to be recorded and processed, and drastically reduces the computational time of the reconstruction. Experimentally we measure the tempo…
We theoretically study a novel approach for soliton-induced high-power supercontinuum generation by using kagome lattice HC-PCFs filled with a noble gas. Anomalous dispersion and broad-band low loss of these fibers enable the generation of two-octave broad spectra by fs pulses, with high coherence and high spectral peak power densities up to five orders of magnitude larger than in standard PCFs. In addition, up to 20 percents of the output radiation energy forms a narrow UV/VUV band, which can be tuned by contolling the pressure in the range from 350 nm to 120 nm. In the temporal domain this c…
We report on the generation of intense extreme ultraviolet (EUV) supercontinuum with photon energies spanning from 35 eV to 50 eV (i. e., supporting an isolated attosecond pulse with a duration of ~271 as) by loosely focusing 35 fs, 11 mJ pulses from a femtosecond laser amplifier into a 10-mm long gas cell filled with krypton gas. The dramatic change of spectral and temporal properties of the driver pulses after passing through the gas cell indicates that propagation effects play a significant role in promoting the generation of the EUV supercontinuum.
We study theoretically the propagation of relatively long pulses with ionizing intensities in a hollow-core photonic crystal fiber filled with a Raman-inactive gas. Due to photoionization, previously unknown types of asymmetric self-phase modulation and `universal' modulational instabilities existing in both normal and anomalous dispersion regions appear. We also show that it is possible to spontaneously generate a plasma-induced continuum of blueshifting solitons, opening up new possibilities for pushing supercontinuum generation towards shorter and shorter wavelengths.
Supercontinuum (SC) light source has advanced ultrafast laser spectroscopy in condensed matter science, biology, physics, and chemistry. Compared to the frequently used photonic crystal fibers and bulk materials, femtosecond laser filamentation in gases is damage-immune for supercontinuum generation. A bottleneck problem is the strong jitters from filament induced self-heating at kHz repetition rate level. We demonstrate stable kHz supercontinuum generation directly in air with multiple mJ level pulse energy. This is achieved by applying an external DC electric field to the air plasma filament…
We demonstrate efficient generation of coherent super-octave pulses via a single-stage spectral broadening of a Yb:KGW laser in a single, pressurized, Ne-filled, hollow-core fiber capillary. Emerging pulses spectrally spanning over more than $\sim$1 PHz (250 nm- 1600 nm) at a dynamic range of $\sim$60 dB, and an excellent beam quality open the door to combining Yb:KGW lasers with modern light field synthesis techniques. Compression of a fraction of the generated supercontinuum to intense (8 fs, $\sim$2.4 cycle, $\sim$650 $μ$J) pulses allows convenient use of these novel laser sources in strong…
Spectral anti-crossings between the fundamental guided mode and core wall resonances alter the dispersion in hollow-core anti-resonant-reflection photonic crystal fibers. Here we study the effect of this dispersion change on the nonlinear propagation and dynamics of ultrashort pulses. We find that it causes emission of narrow spectral peaks through a combination of four-wave mixing and dispersive wave emission. We further investigate the influence of the anti-crossings on nonlinear pulse propagation and show that their impact can be minimized by adjusting the core-wall thickness in such a way …
Ultraviolet frequency combs enable applications ranging from precision spectroscopy to atomic clocks by addressing the electronic transitions of atoms and molecules. Access to ultraviolet light via integrated nonlinear optics is usually hampered by the strong material dispersion and large waveguide attention in the ultraviolet region. Here we demonstrate a simple route to chip-scale ultraviolet comb generators, simultaneously showing a gap-free frequency span of ~128 terahertz and supercontinuum sourced by an ultrafast fiber laser. The simultaneous cubic and quadratic nonlinear processes are i…
Oscillator-driven broadband femtosecond transient microspectroscopy with supercontinuum probes generated in a photonic crystal fiber
Osaka Metropolitan University（大阪公立大学）；Institute for Molecular Science, National Institutes of Natural Sciences（国立自然科学研究所分子科学研究所）；Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC)（马德里材料科学研究所）
Single-shot supercontinuum spectral interferometry (SSSI) is an optical technique that can measure ultrafast transients in the complex index of refraction. This method uses chirped supercontinuum reference/probe pulses that need to be pre-characterized prior to use. Conventionally, the spectral phase (or chirp) of those pulses can be determined from a series of phase or spectral measurements taken at various time delays with respect to a pump-induced modulation. Here we propose a novel method to simplify this process and characterize reference/probe pulses up to the third order dispersion from…
We report generation of an ultrafast supercontinuum extending into the mid- infrared in gas-filled single-ring hollow-core photonic crystal fiber (SR-PCF) pumped by 1.7 $μ$m light from an optical parametric amplifier. The simple fiber structure offers shallow dispersion and flat transmission in the near and mid-infrared, enabling the generation of broadband spectra extending from 300 nm to 3.1 $μ$m, with a total energy of a few $μ$J. In addition, we report the emission of ultraviolet dispersive waves whose frequency can be tuned simply by adjusting the pump wavelength. SR-PCF also provides an …
Controlling femtosecond optical pulses with temporal precision better than one cycle of the carrier field has a profound impact on measuring and manipulating interactions between light and matter. We explore pulses that are carved from a continuous-wave laser via electro-optic modulation and realize the regime of sub-cycle optical control without a mode-locked resonator. Our ultrafast source, with a repetition rate of 10 GHz, is derived from an optical-cavity-stabilized laser and a microwave-cavity-stabilized electronic oscillator. Sub-cycle timing jitter of the pulse train is achieved by cohe…
The physics and applications of fiber-based supercontinuum (SC) sources have been a subject of intense interest over the last decade, with significant impact on both basic science and industry. New uses for SC sources are also constantly emerging due to their unique properties that combine high brightness, multi-octave frequency bandwidth, fiber delivery, and single-mode output. The last few years have seen significant research efforts focused on extending the wavelength coverage of SC sources towards the 2 to 20 $μ$m molecular fingerprint mid-infrared (MIR) region and in the ultraviolet (UV) …
We report a novel source of twin beams based on modulational instability in high-pressure argon-filled hollow-core kagomé-style photonic-crystal fibre. The source is Raman-free and manifests strong photon-number correlations for femtosecond pulses of squeezed vacuum with a record brightness of ~2500 photons per mode. The ultra-broadband (~50 THz) twin beams are frequency tunable and contain one spatial and less than 5 frequency modes.
The field of attosecond science was first enabled by nonlinear compression of intense laser pulses to a duration below two optical cycles. Twenty years later, creating such short pulses still requires state-of-the-art few-cycle laser amplifiers to most efficiently exploit 'instantaneous' optical nonlinearities in noble gases for spectral broadening and parametric frequency conversion. Here, we show that nonlinear compression can in fact be much more efficient when driven in molecular gases by pulses substantially longer than a few cycles, due to enhanced optical nonlinearity associated with ro…
We investigate numerically soliton-plasma interaction in a noble-gas-filled silica hollow-core anti-resonant fiber pumped in the mid-IR at 3.0 μm. We observe multiple soliton self-compression stages due to distinct stages where either the self-focusing or the self-defocusing nonlinearity dominates. Specifically, the parameters may be tuned so the competing plasma self-defocusing nonlinearity only dominates over the Kerr self-focusing nonlinearity around the soliton self-compression stage, where the increasing peak intensity on the leading pulse edge initiates a competing self-defocusing plasma…
The propagation of ultrashort pulses in optical fibre displays complex nonlinear dynamics that find important applications in fields such as high power pulse compression and broadband supercontinuum generation. Such nonlinear evolution however, depends sensitively on both the input pulse and fibre characteristics, and optimizing propagation for application purposes requires extensive numerical simulations based on generalizations of a nonlinear Schrödinger-type equation. This is computationally-demanding and creates a severe bottleneck in using numerical techniques to design and optimize exper…
We vary the time-frequency mode structure of ultrafast pulse-pumped modulational instability (MI) twin beams in an argon-filled hollow-core kagomé-style PCF by adjusting the pressure, pump pulse chirp, fiber length and parametric gain. Compared to solid-core systems, the pressure dependent dispersion landscape brings increased flexibility to the tailoring of frequency correlations and we demonstrate that the pump pulse chirp can be used to tune the joint spectrum of femtosecond-pumped sources. We also characterize the resulting mode content, not only by measuring the multimode second-order cor…
We present the results of an experimental and numerical investigation into temporally non-local coherent interactions between ultrashort pulses, mediated by Raman coherence, in gas-filled kagomé-style hollow-core photonic crystal fiber. A pump pulse first set up the Raman coherence, creating a refractive index grating in the gas that travels at the group velocity of the pump pulse. Varying the arrival time of a second probe pulse allows high degree of control over its evolution as it propagates along the fiber, in particular soliton self-compression and dispersive wave (DW) emission. In the ex…
We present a table-top beamline providing a soft X-ray supercontinuum extending up to 350 eV from high-order harmonic generation with sub-13 fs 1300 nm driving pulses and simultaneous production of sub-5 fs pulses centered at 800 nm. Optimization of the high harmonic generation in a long and dense gas medium yields a photon flux of ~2 x 10^7 photons/s/1% bandwidth at 300 eV. The temporal resolution of X-ray transient absorption experiments with this beamline is measured to be 11 fs for 800 nm excitation. This dual-wavelength approach, combined with high flux and high spectral and temporal reso…
Mid-infrared-to-ultraviolet supercontinuum generation in low-loss tantalum pentoxide nanophotonic waveguides
State Key Laboratory of Ultra-intense Laser Science and Technology, Shanghai Institute of Optics and Fine Mechanics, Chinese Academy of Sciences（中国科学院上海光学精密机械研究所）；Key Laboratory of Specialty Fiber Optics and Optical Access Networks, Shanghai University（上海大学）；The Extreme Optoelectromechanics Laboratory (XXL), School of Physics, East China Normal University（华东师范大学）；State Key Laboratory of Precision Spectroscopy, East China Normal University（华东师范大学）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学）；University College London（伦敦大学学院）；Shanghai Research Center for Quantum Sciences（上海量子科学研究中心）；Hefei National Laboratory（合肥国家实验室）；Collaborative Innovation Center of Extreme Optics, Shanxi University（山西大学）；Collaborative Innovation Center of Light Manipulations and Applications, Shandong Normal University（山东师范大学）
We propose a Watt-level, all-fiber, ultrafast Er/Yb-codoped double-clad fiber laser passively mode-locked by reduced graphene oxide (rGO) interacting with a weak evanescent field of photonic crystal fiber (PCF). The rGO solution is filled into the cladding holes of the PCF based on total reflection, and after evaporation, the rGO flakes bear only 1/107 of the total energy in laser system, which enhances the thermal damage threshold and decreases the accumulated nonlinearity. By incorporating the saturable absorber into an Er/Yb-codoped fiber ring cavity, stable conventional soliton with a dura…
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 dispe…
We present a pump-probe technique for monitoring ultrafast polarizability changes. In particular, we use it to measure the plasma density created at the temporal focus of a self-compressing higher-order pump soliton in gas-filled hollow-core photonic crystal fiber. This is done by monitoring the wavelength of the dispersive wave emission from a counter-propagating probe soliton. By varying the relative delay between pump and probe, the plasma density distribution along the fiber can be mapped out. Compared to the recently introduced interferometric side-probing for monitoring the plasma densit…
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. Bas…
We report generation of a femtosecond supercontinuum extending from the ultraviolet to the near-infrared and detection of its carrier-envelope phase variation by f-to-2f interferometry. The spectrum is generated in a gas-filled hollow-core photonic crystal fiber where soliton dynamics allows CEP-stable self-compression of OPCPA pump pulses at 800 nm to a duration of 1.7 optical cycles, followed by dispersive wave emission. The source provides up to 1 μJ of pulse energy at 800 kHz repetition rate resulting in 0.8 W of average power, and can be extremely useful for example in strong-field physic…
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 inter…
