Ultrafast 1 MHz vacuum-ultraviolet source via highly cascaded harmonic generation in negative-curvature hollow-core fibers
David E. Couch, Daniel D. Hickstein, David G. Winters, Sterling J. Backus, Matthew S. Kirchner, Scott R. Domingue, Jessica J. Ramirez, Charles G. Durfee, Margar… 展开作者
David E. Couch, Daniel D. Hickstein, David G. Winters, Sterling J. Backus, Matthew S. Kirchner, Scott R. Domingue, Jessica J. Ramirez, Charles G. Durfee, Margaret M. Murnane, Henry C. Kapteyn
Vacuum ultraviolet (VUV) light is critical for the study of molecules and materials, but the generation of femtosecond pulses in the VUV region at high repetition rates has proven difficult. Here, we demonstrate the efficient generation of VUV light at MHz repetition rates using highly cascaded four-wave mixing processes in a negative-curvature hollow-core fiber. Both even and odd order harmonics are generated up to the 15th harmonic (69 nm, 18.0 eV), with high energy resolution of ~40 meV. In contrast to direct high harmonic generation, this highly cascaded harmonic generation process requires lower peak intensity and therefore can operate at higher repetition rates, driven by a robust ~10 W fiber-laser system in a compact setup. Additionally, we present numerical simulations that explore the fundamental capabilities and spatiotemporal dynamics of highly cascaded harmonic generation. This VUV source can enhance the capabilities of spectroscopies of molecular and quantum materials, such as photoionization mass spectrometry and time , angle , and spin-resolved photoemission.
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…
Cascaded nonlinearities have attracted much interest, but ultrafast applications have been seriously hampered by the simultaneous requirements of being near phase-matching and having ultrafast femtosecond response times. Here we show that in strongly phase-mismatched nonlinear frequency conversion crystals the pump pulse can experience a large and extremely broadband self-defocusing cascaded Kerr-like nonlinearity. The large cascaded nonlinearity is ensured through interaction with the largest quadratic tensor element in the crystal, and the strong phase-mismatch ensures an ultrafast nonlinear…
We demonstrate, for the first time, the application of rare-gas filled hollow-core photonic crystal fibres (HC-PCFs) as tuneable ultraviolet light sources in femtosecond pump-probe spectroscopy. The time-resolved photoelectron imaging technique reveals non-adiabatic dynamical processes operating on three distinct timescales in the styrene molecule following excitation over the 242-258 nm region. These include ultrafast (<100 fs) internal conversion between the S2(pipi*) and S1(pipi*) electronic states and subsequent intramolecular vibrational energy redistribution within S1(pipi*). Compact, co…
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 …
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…
Hollow Gaussian beams (HGB) are a special class of doughnut shaped beams that do not carry orbital angular momentum (OAM). Such beams have a wide range of applications in many fields including atomic optics, bio-photonics, atmospheric science, and plasma physics. Till date, these beams have been generated using linear optical elements. Here, we show a new way of generating HGBs by three-wave mixing in a nonlinear crystal. Based on nonlinear interaction of photons having OAM and conservation of OAM in nonlinear processes, we experimentally generated ultrafast HGBs of order as high as 6 and powe…
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 investigate various methods for extending the simple analytical capillary model to describe the dispersion and loss of anti-resonant hollow-core fibers without the need of detailed finite-element simulations across the desired wavelength range. This poor-man's model can with a single fitting parameter quite accurately mimic dispersion and loss resonances and anti-resonances from full finite-element simulations. Due to the analytical basis of the model it is easy to explore variations in core size and cladding wall thickness, and should therefore provide a valuable tool for numerical simulat…
Simple structures are always a pursuit but sometimes not easily attainable. It took researchers nearly two decades for conceiving the structure of single-ring hollow-core negative curvature fiber (NCF). Recently NCF eventually approaches to the centre of intense study in fiber optics. The reason behind this slow-pace development is, undoubtfully, its inexplicit guidance mechanism. This paper aims at gaining a clear physical insight into the optical guidance mechanism in NCF. To clarify the origins of light confinement, we boldly disassemble the NCF structure into several layers and develop a m…
A flexible and accurate total variation and cascaded denoisers-based image reconstruction algorithm for hyperspectrally compressed ultrafast photography
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 c…
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…
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 a…
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 …
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 …
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.
When ultrafast noncritical cascaded second-harmonic generation of energetic femtosecond pulses occur in a bulk lithium niobate crystal optical Cherenkov waves are formed in the near- to mid-IR. Numerical simulations show that the few-cycle solitons radiate Cherenkov (dispersive) waves in the $λ=2.2-4.5\mic$ range when pumping at $λ_1=1.2-1.8\mic$. The exact phase-matching point depends on the soliton wavelength, and we show that a simple longpass filter can separate the Cherenkov waves from the solitons. The Cherenkov waves are born few-cycle with an excellent Gaussian pulse shape, and the con…
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…
High-energy ultraviolet pulse generation in gas-filled hollow capillary fibers (HCFs) through dispersive-wave-emission process, has attracted considerable attentions in recent several years due to its great application potentials in ultraviolet spectroscopy and photochemistry. While the ability of this technique to deliver high-energy, ultrafast ultraviolet pulses is widely recognized, few-fs duration of μJ-level dispersive-wave (DW) pulses has, however, escaped direct measurements. In this letter, we demonstrate that using several chirped mirrors, few-fs ultraviolet DW pulses can be obtained …
Metasurfaces control optical wavefronts via arrays of nanoscale resonators laid out across a surface. When combined with III-V semiconductors with strong optical nonlinearities, a variety of nonlinear effects such as harmonic generation and all optical modulation can be enabled and enhanced at the nanoscale. This review presents our research on engineering and boosting nonlinear effects in ultrafast and nonlinear semiconductor metasurfaces fabricated at the Center for Integrated Nanotechnologies (CINT). We cover our recent works on parametric generation of harmonic light via direct and cascade…
Modeling and Optimization of Cascaded Four-Wave Mixing toward the VUV in Xenon-Filled Negative-Curvature Fibers
Gleb Wataghin Institute of Physics, University of Campinas – UNICAMP（坎皮纳斯大学 Gleb Wataghin 物理研究所）；GPPMM Group, XLIM Institute, CNRS UMR 7252, University of Limoges（利摩日大学 XLIM 研究所 GPPMM 研究组）；Multiuser Laboratory of Optics and Photonics, LaMOF, Federal University of Lavras（拉夫拉斯联邦大学 LaMOF 光学与光子学多用户实验室）
The possibility of performing time-resolved spectroscopic studies in the molecular fingerprinting region or extending the cut-off wavelength of high-harmonic generation has recently boosted the development of efficient mid-infrared ultrafast lasers. In particular, fibre lasers based on active media such as thulium or holmium are a very active area of research since they are robust, compact and can operate at high repetition rates. These systems, however, are still complex, are unable to deliver pulses shorter than 100 fs and are not yet as mature as their near-infrared counterparts. Here we re…
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…
Gas-filled hollow-core fiber (HCF) pulse post-compressors generating few- to single-cycle pulses are a key enabling tool for attosecond science and ultrafast spectroscopy. Achieving optimum performance in this regime can be extremely challenging due to the ultra-broad bandwidth of the pulses and the need of an adequate temporal diagnostic. These difficulties have hindered the full exploitation of HCF post-compressors, namely the generation of stable and high-quality near-Fourier-transform-limited pulses. Here we show that, independently of conditions such as the type of gas or the laser system…
The resonance band in hollow-core photonic crystal fiber (HC-PCF), while leading to high-loss region in the fiber transmission spectrum, has been successfully used for generating phase-matched dispersive wave (DW). Here, we report that the spectral width of the resonance-induced DW can be largely broadened due to plasma-driven blueshifting soliton. In the experiment, we observed that in a short length of Ar-filled single-ring HC-PCF the soliton self-compression and photoionization effects caused a strong spectral blueshift of the pump pulse, changing the phase-matching condition of the DW emis…
Recently, Grange et al. [Phys. Rev. Lett. 114, 193601 (2015)] showed the possibility of single photon generation with high indistinguishability from a quantum emitter, despite strong pure dephasing, by `funneling' emission into a photonic cavity. Here, we show that cascaded two-cavity system can further improve the photon characteristics and greatly reduce the Q-factor requirement to levels achievable with present-day technology. Our approach leverages recent advances in nanocavities with ultrasmall mode volume and does not require ultrafast excitation of the emitter. These results were obtain…
We propose a scheme for the emission of few-cycle dispersive waves in the mid-infrared using hollow-core photonic crystal fibers filled with noble gas. The underlying mechanism is the formation of a plasma cloud by a self-compressed, sub-cycle pump pulse. The resulting free-electron population modifies the fiber dispersion, allowing phase-matched access to dispersive waves at otherwise inaccessible frequencies, well into the mid-IR. Remarkably, the pulses generated turn out to have durations of the order of two optical cycles. In addition, this ultrafast emission, which occurs even in the abse…
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 $μ$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 …
Ultrashort high-energy pulses at wavelengths longer than 1 $μ$m are nowadays desired for a vast variety of applications in ultrafast and strong-field physics. To date, the main answer to the wavelength tunability for energetic, broadband pulses still relies on optical parametric amplification (OPA), which often requires multiple and complex stages, may feature imperfect beam quality and has limited conversion efficiency into one of the amplified waves. In this work, we present a completely different strategy to realize an energy-efficient and scalable laser frequency shifter. This relies on th…
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…
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 genera…
Antisymmetric chirp transfer to high-energy ultraviolet pulses via gas-based chirped four-wave mixing
University of California Los Angeles（加州大学洛杉矶分校）；California NanoSystems Institute（加州纳米系统研究所）；SLAC National Accelerator Laboratory, Stanford University（斯坦福大学SLAC国家加速器实验室）
Low-threshold efficient N${_2^+}$ lasing driven by sub-cycle soliton dynamics in a hollow waveguide
State Key Laboratory of Ultra-intense Laser Science and Technology, Shanghai Institute of Optics and Fine Mechanics (SIOM), Chinese Academy of Sciences (CAS)（中国科学院上海光学精密机械研究所超强度激光科学与技术国家重点实验室）；Russell Centre for Advanced Lightwave Science, Shanghai Institute of Optics and Fine Mechanics (SIOM) and Hangzhou Institute of Optics and Fine Mechanics (HIOM)（上海光学精密机械研究所与杭州光学精密机械研究所先进光波科学中心）；Zhejiang Key Laboratory of Microstructured Specialty Optical Fiber, Hangzhou Institute of Optics and Fine Mechanics (HIOM)（杭州光学精密机械研究所微结构特种光纤浙江省重点实验室）；School of Optoelectronic Engineering, Xidian University（西安电子科技大学光电工程学院）；School of Optical-Electrical and Computer Engineering, University of Shanghai for Science and Technology（上海理工大学光电信息与计算机工程学院）；Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences（中国科学院大学杭州高等研究院）；Zhangjiang Laboratory（张江实验室）
Generating energetic femtosecond mid-IR pulses is crucial for ultrafast spectroscopy, and currently relies on parametric processes that, while efficient, are also complex. Here we experimentally show a simple alternative that uses a single pump wavelength without any pump synchronization and without critical phase-matching requirements. Pumping a bulk quadratic nonlinear crystal (unpoled LiNbO$_3$ cut for noncritical phase-mismatched interaction) with sub-mJ near-IR 50-fs pulses, tunable and broadband ($\sim 1,000$ cm$^{-1}$) mid-IR pulses around $3.0~μ\rm m$ are generated with excellent spati…
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…
Technical design report of a complete and compact broadband high-harmonics femtosecond beamline based on a modular hollow waveguide for photons generation centered on the upper region of the extreme ultraviolet spectral range
Institut de Physique et Chimie des Materiaux, CNRS, IPCMS, UMR 7504（材料物理与化学研究所）；Université de Caen Normandie, ENSICAEN, CNRS/IN2P3, LPC Caen UMR6534（卡昂诺曼底大学）
Tailoring optical nonlinear effects (e.g. harmonic generation, sum-frequency mixing, etc.) in the recently emerging all-dielectric platform is important for both the fundamental science and industrial development of high-efficiency, ultrafast, and miniaturized photonic devices. In this work, we propose a novel paradigm for dynamically switchable high-harmonic generation in Silicon nanodimer metasurfaces by exploiting polarization-controlled dual bound states in the continuum (BIC). Owing to the high-quality factor of BIC resonances, efficient harmonic signals including the third-harmonic gener…
We present nonlinear pulse compression of a high-power SESAM-modelocked thin-disk laser (TDL) using an Ar-filled hypocycloid-core Kagome Hollow-Core Photonic Crystal Fiber (HC-PCF). The output of the modelocked Yb:YAG TDL with 127 W average power, a pulse repetition rate of 7 MHz, and a pulse duration of 740 fs was spectrally broadened 16-fold while propagating in a Kagome HC-PCF containing 13 bar of static Argon gas. Subsequent compression tests performed using 8.4% of the full available power resulted in a pulse duration as short as 88 fs using the spectrally broadened output from the fiber.…
We propose and experimentally demonstrate a novel experimental scheme to generate high peak power, segmented, smooth, zero-order Bessel beams with tunable range. Illuminating the axicon with hollow Gaussian beams (HGBs) of different orders we have generated Bessel beams of varying range at different positions away from the axicon. The presence of dark core at the center of the HGBs removes the effect of imperfection in the axicon tip. As a result, the entire power of the input beam is transformed into zero-order Bessel beam without any on-axis intensity modulation. We observe the decrease in r…
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) …
Novel table-top sources of extreme-ultraviolet light based on high-harmonic generation yield unique insight into the fundamental properties of molecules, nanomaterials, or correlated solids, and enable advanced applications in imaging or metrology. Extending high-harmonic generation to high repetition rates portends great experimental benefits, yet efficient extreme-ultraviolet conversion of correspondingly weak driving pulses is challenging. Here, we demonstrate a highly efficient source of femtosecond extreme-ultraviolet pulses at 50-kHz repetition rate, utilizing the ultraviolet second-harm…
