The unique ring-shaped intensity patterns and helical phase fronts of optical vortices make them useful in many applications. Here we report for the first time efficient Raman frequency conversion between vortex modes in twisted hydrogen-filled single-ring hollow core photonic crystal fiber (SR-PCF). High fidelity transmission of optical vortices in untwisted SR-PCF becomes more and more difficult as the orbital angular momentum (OAM) order increases, due to scattering at structural imperfections in the fiber microstructure. In helically twisted SR-PCF, however, the degeneracy between left- and right-handed versions of the same mode is lifted, with the result that they are topologically protected from such scattering. With launch efficiencies of ~75%, a high damage threshold and broadband guidance, these fibers are ideal for performing nonlinear experiments that require the polarization state and azimuthal order of the interacting modes to be preserved over long distances. Vortex coherence waves (VCW) of internal molecular motion, carrying angular momentum, are excited in the gas, permitting the polarization and orbital angular momentum of the Raman bands to be tailored, even in spectral regions where conventional solid-core waveguides are opaque or susceptible to optical damage.
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…
In this letter, the characteristics of noise and long-term stability of near- and mid-infrared (near-IR and mid-IR) gas-filled fiber Raman lasers have been investigated for the first time. The results reveal that an increase in Raman pulse energy is associated with a decrease in noise, and that the relative pulse peak intensity noise (RIN) is always lower than the relative pulse energy noise (REN). We also demonstrate that long-term drift of the pulse energy and peak power are directly linked with the high amount of heat release during the Raman Stokes generation. The demonstrated noise and lo…
We report the generation of a purely vibrational Raman comb, extending from the vacuum ultraviolet (184 nm) to the visible (478 nm), in hydrogen-filled kagomé-style photonic crystal fiber pumped at 266 nm. Stimulated Raman scattering and molecular modulation processes are enhanced by higher Raman gain in the ultraviolet. Owing to the pressure-tunable normal dispersion landscape of the fiber-gas system in the ultraviolet, higher-order anti-Stokes bands are generated preferentially in higher-order fiber modes. The results pave the way towards tunable fiber-based sources of deep- and vacuum ultra…
We have developed an analytical model based on the perturbation theory in order to study the optical propagation of two successive intense solitons in hollow-core photonic crystal fibers filled with Raman-active gases. Based on the time delay between the two solitons, we have found that the trailing soliton dynamics can experience unusual nonlinear phenomena such as spectral and temporal soliton oscillations and transport towards the leading soliton. The overall dynamics can lead to a spatiotemporal modulation of the refractive index with a uniform temporal period and a uniform or chirped spat…
In this work, we present a high pulse energy multi-wavelength Raman laser spanning from 1.53 um up to 2.4 um by employing the cascaded rotational stimulated Raman scattering (SRS) effect in a 5-m hydrogen (H2) -filled nested anti-resonant fiber (NARF), pumped by a linearly polarized Er/Yb fiber laser with a peak power of ~13 kW and pulse duration of ~7 ns in the C-band. The developed Raman laser has distinct lines at 1683 nm, 1868 nm, 2100 nm, and 2400 nm, with pulse energies as high as 18.25 uJ, 14.4 uJ, 14.1 uJ, and 8.2 uJ, respectively. We demonstrate how the energy in the Raman lines can b…
As shown in the early 1960s, the gain in stimulated Raman scattering (SRS) is drastically suppressed when the rate of creation of phonons (via pump-to-Stokes conversion) is exactly balanced by the rate of phonon annihilation (via pump-to-anti-Stokes conversion). This occurs when the phonon coherence waves synchronized vibrations of a large population of molecules have identical propagation constants for both processes, i.e., they are phase-velocity matched. As recently demonstrated, hydrogen-filled photonic crystal fiber pumped in the vicinity of its zero dispersion wavelength provides an idea…
Optical properties of hollow-core revolver fibers are numerically investigated depending on various parameters: the hollow-core diameter, the capillary wall thickness, the values of the minimum gap between the capillaries, the number of capillaries in the cladding and the type of glass (silica and chalcogenide). Preliminary, similar calculations are made for simple models of hollow-core fibers. Based on the obtained results, the optimal design of the revolver fiber for Raman laser frequency conversion (1560 nm to 4420 nm in H2) was determined. As a result, efficient ns-pulsed 4420 nm Raman las…
Coherent ultraviolet (UV) light has many uses, for example in the study of molecular species relevant in biology and chemistry. Very few if any laser materials offer UV transparency along with damage-free operation at high photon energies and laser power. Here we report efficient generation of deep and vacuum UV light using hydrogen-filled hollow-core photonic crystal fiber (HC-PCF). Pumping above the stimulated Raman threshold at 532 nm, coherent molecular vibrations are excited in the gas, permitting highly efficient thresholdless wavelength conversion in the UV. The system is uniquely press…
In 1964 Bloembergen and Shen predicted that Raman gain could be suppressed if the rates of phonon creation and annihilation (by inelastic scattering) exactly balance. This is only possible if the momentum required for each process is identical, i.e., phonon coherence waves created by pump-to-Stokes scattering are identical to those annihilated in pump-to-anti-Stokes scattering. In bulk gas cells, this can only be achieved over limited interaction lengths at an oblique angle to the pump axis. Here we report a simple system that provides dramatic Raman gain suppression over long collinear path-l…
Broadband-tunable sources of circularly-polarized light are crucial in fields such as laser science, biomedicine and spectroscopy. Conventional sources rely on nonlinear wavelength conversion and polarization control using standard optical components, and are limited by the availability of suitably transparent crystals and glasses. Although gas-filled hollow-core photonic crystal fiber provides pressure-tunable dispersion, long well-controlled optical path-lengths, and high Raman conversion efficiency, it is unable to preserve circular polarization state, typically exhibiting weak linear biref…
We propose supercritical xenon in a hollow-core photonic bandgap fiber as a highly nonlinear medium, and demonstrate 200 nm control over the guidance window of the fiber as the xenon goes through its supercritical phase transition. The large optical polarizability and monoatomic nature of xenon are predicted to allow large optical nonlinearity, on the same order as that of fused silica, while maintaining greatly reduced Raman scattering, offering benefits for nonlinear and quantum optics.
Many fields such as bio-spectroscopy and photochemistry often require sources of vacuum ultraviolet (VUV) pulses featuring a narrow linewidth and tunable over a wide frequency range. However, the majority of available VUV light sources do not simultaneously fulfill those two requirements, and few if any are truly compact, cost-effective and easy to use by non-specialists. Here we introduce a novel approach that goes a long way to meeting this challenge. It is based on hydrogen-filled hollow-core photonic crystal fiber pumped simultaneously by two spectrally distant pulses. Stimulated Raman sca…
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.
Backward stimulated Raman scattering in gases provides a promising route to compression and amplification of a Stokes seed-pulse by counter-propagating against a pump-pulse, as has been already demonstrated in various platforms, mainly in free-space. However, the dynamics governing this process when seeded by noise has not yet been investigated in a fully controllable collinear environment. Here we report the first unambiguous observation of efficient noise-seeded backward stimulated Raman scattering in a hydrogen-filled hollow-core photonic crystal fiber. At high gas pressures, when the backw…
Using an example of a Raman active medium we describe how a common nonlinear process of four-wave mixing can be used to induce strong coupling between the spatial and temporal degrees of freedom in optical waves. This coupling produces several unexpected effects. Amongst those are cascaded excitation of multiply charged optical vortices, spatial focusing in a nonlinearly defocusing medium and generation of helically shaped spatio-temporal optical solitons.
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 study the formation of off-axis optical vortices propagating inside a double-Raman gain atomic medium. The atoms interact with two weak probe fields as well as two strong pump beams which can carry orbital angular momentum (OAM). We consider a situation when only one of the strong pump lasers carries an OAM. A particular superposition of probe fields coupled to the matter is shown to form specific optical vortices with shifted axes. Such off-axis vortices can propagate inside the medium with sub- or superluminal group velocity depending on the value of the two-photon detuning. The superlumi…
In this paper we consider mid-infrared Raman lasers based on gas-filled hollow-core silica fibers and provide theoretical and experimental analysis of factors that limit the efficiency and output power of these lasers. As a result, we realized an efficient ns-pulsed 4.42 μm Raman laser based on an 1H2-filled revolver silica fiber. Quantum efficiency as high as 36 % is achieved, and output average power as high as 250 mW is demonstrated. The possibilities of further improving the laser efficiency are discussed.
We study coherent anti-Stokes Raman spectroscopy in air-filled anti-resonance hollow-core photonic crystal fiber, otherwise known as 'revolver' fiber. We compare the vibrational coherent anti-Stokes Raman signal of N$_2$, at 2331 cm$^{-1}$, generated in ambient air (no fiber present), with the one generated in a 2.96 cm of a revolver fiber. We show a 170 times enhancement for the signal produced in the fiber, due to an increased interaction path. Remarkably, the N$_2$ signal obtained in the revolver fiber shows near-zero non-resonant background, due to near-zero overlap between the laser field…
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…
We report a study of soliton self-frequency shifting in hydrogen-filled hollow-core fiber. The combination of hydrogen and short 40-fs input pulses underlies clean and efficient generation of Raman solitons between 1080 and 1600 nm. With 240-nJ input pulses, the Raman soliton energy ranges from 110 to 20 nJ over that wavelength range, and the pulse duration is approximately 45 fs. In particular, 70-nJ and 42-fs pulses are generated at 1300 nm. Numerical simulations agree reasonably well with experiments and predict that microjoule-energy tunable pulses should be possible with higher-energy inp…
Based on the interplay between photoionization and Raman effect in gas-filled photonic crystal fibers, we propose a new optical device to control frequency-conversion of ultrashort pulses. By tuning the input-pulse energy, the output spectrum can be either down-converted, up-converted, or even frequency-shift compensated. For low input energies, Raman effect is dominant and leads to a redshift that increases linearly during propagation. For larger pulse energies, photoionization starts to take over the frequency conversion process, and induces a strong blueshift. We have found also that the fi…
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…
We report a novel scheme for the generation of dense clusters of Raman sidebands. The scheme uses a broadband-guiding hollow-core photonic crystal fiber (HC-PCF) filled with a mixture of H2, D2, and Xe for efficient interaction between the gas mixture and a green laser pump pulse (532 nm, 1 ns) of only 5 uJ energy. This results in the generation from noise of more than 135 ro-vibrational Raman sidebands covering the visible spectral region with an average spacing of only 2 THz. Such a spectrally dense and compact fiber-based source is ideal for applications where closely spaced narrow-band las…
When a laser pump beam of sufficient intensity is incident on a Raman-active medium such as hydrogen gas, a strong Stokes signal, red-shifted by the Raman transition frequency Ω$_R$, is generated. This is accompanied by the creation of a "coherence wave" of synchronized molecular oscillations with wavevector Δβ determined by the optical dispersion. Within its lifetime, this coherence wave can be used to shift by Ω$_R$ the frequency of a third "mixing" signal, provided phase-matching is satisfied, i.e., Δβ is matched. Conventionally this can be arranged using non-collinear beams or higher-order…
We propose an optical trapping technique in which a fundamental soliton traps an ultrashort small amplitude radiation in a symmetric hollow-core photonic crystal fiber filled with a noble gas, preventing its dispersion. The system is Raman- and plasma-free. Trapping is due to the cross phase modulation effect between the two pulses. The trapped radiation inside the soliton-induced potential will oscillate periodically due to the shock effect, similar to the motion of a mechanical pendulum.
We report on two types of Raman laser sources emitting in the near and middle ultraviolet spectral ranges by the use of a solarization-resilient gas-filled inhibited-coupling (IC) hollow-core photonic-crystal fiber (HCPCF) with record low transmission loss (minimum of 5 dB/km at 480 nm). The first source type emits a Raman comb generated in a hydrogen-filled HCPCF pumped by a 355 nm wavelength microchip nanosecond pulsed laser. The generated comb lines span from 270 nm to the near-infrared region with no less than 20 lines in the 270-400 nm wavelength range. The second type stands for the firs…
We show theoretically that the photoionization process in a hollow-core photonic crystal fiber filled with a Raman-inactive noble gas leads to a constant acceleration of solitons in the time domain with a continuous shift to higher frequencies, limited only by ionization loss. This phenomenon is opposite to the well-known Raman self-frequency red-shift of solitons in solid-core glass fibers. We also predict the existence of unconventional long-range non-local soliton interactions leading to spectral and temporal soliton clustering. Furthermore, if the core is filled with a Raman-active molecul…
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.
We present a technique that uses noisy broadband pulse bursts generated by modulational instability to probe nonlinear processes, including infrared-inactive Raman transitions, in molecular gases. These processes imprint correlations between different regions of the noisy spectrum, which can be detected by acquiring single shot spectra and calculating the Pearson correlation coefficient between the different frequency components. Numerical simulations verify the experimental measurements and are used to further understand the system and discuss methods to improve the signal strength and the sp…
Supercritical Xe at 293 K offers a Kerr nonlinearity that can exceed that of fused silica while being free of Raman scattering. It also has a much higher optical damage threshold and a transparency window that extends from the UV to the infrared. We report the observation of nonlinear phenomena, such as self-phase modulation, in hollow-core photonic crystal fiber filled with supercritical Xe. In the subcritical regime, intermodal four-wave-mixing resulted in the generation of UV light in the HE12 mode. The normal dispersion of the fiber at high pressures means that spectral broadening can clea…
In this letter, we present a high pulse energy Raman laser at 1946 nm wavelength directly pumped with a 1533 nm custom-made fiber laser. The Raman laser is based on the stimulated Raman scattering (SRS) in an 8-meter carbon dioxide (CO2) filled nested anti-resonant hollow-core fiber (ARHCF). The low energy phonon emission combined with the inherent SRS process along the low-loss fiber allows the generation of high pulse energy up to 15.4 μJ at atmospheric CO2 pressure. The Raman laser exhibits good long-term stability and low relative intensity noise (RIN) of less than 4%. We also investigate …
We report on experimental and theoretical demonstration of an optical comb spectrum based on a combination of cascaded stimulated Raman scattering and four-wave mixing mediated by Raman-induced nonresonant Kerr-type nonlinearity. This combination enabled to transform a conventional quasi-periodic Raman comb into a comb with a single and smaller frequency spacing. This new phenomenon is realized using a hollow-core photonic crystal fiber filled with 40 bars of deuterium, and pumped with a high-power picosecond laser. The resultant comb shows more than 100 spectral lines spanning over 220 THz fr…
Many reports on stimulated Raman scattering in mixtures of Raman-active and noble gases indicate that the addition of a dispersive buffer gas increases the phase-mismatch to higher-order Stokes and antiStokes sidebands, resulting in preferential conversion to the first few Stokes lines, accompanied by a significant reduction in Raman gain due to collisions with buffer gas molecules. Here we report that, provided the dispersion can be precisely controlled, the effective Raman gain in gas-filled hollow-core photonic crystal fiber (PCF) can actually be significantly enhanced when a buffer gas is …
Highly-efficient perturbative Raman shifting by engineering the nonlinear temporal response
School of Applied and Engineering Physics, Cornell University（康奈尔大学应用工程物理学院）；CREOL, The College of Optics and Photonics, University of Central Florida（中佛罗里达大学光学与光子学院CREOL）
Experimental results from the generation of Raman sidebands using optical vortices are presented. By generating two sets of sidebands originating from different locations in a Raman active crystal, one set containing optical orbital angular momentum and the other serving as a reference, a Young's double slit experiment was simultaneously realized for each sideband. The interference between the two sets of sidebands was used to determine the helicity and topological charge in each order. Topological charges in all orders were found to be discrete and follow selection rules predicted by a cascad…
We predict that a photon condensate inside a dye-filled microcavity forms long-lived spatial structures that resemble vortices when incoherently excited by a focused pump orbiting around the cavity axis. The finely structured density of the condensates have a discrete rotational symmetry that is controlled by the orbital frequency of the pump spot and is phase-coherent over its full spatial extent despite the absence of any effective photon-photon interactions.
We show experimentally and theoretically that the spectral components of a multi-octave frequency comb spontaneously created by stimulated Raman scattering in a hydrogen-filled hollow-core photonic crystal fiber exhibit strong self coherence and mutual coherence within each 12 ns driving laser pulse. This coherence arises in spite of the field's initiation being from quantum zero-point fluctuations, which causes each spectral component to show large phase and energy fluctuations. This points to the possibility of an optical frequency comb with nonclassical correlations between all comb lines.
We report generation of ultrashort UV pulses by soliton self-compression in kagomé-style hollow-core photonic crystal fiber filled with ambient air. Pump pulses with energy 2.6 uJ and duration 54 fs at 400 nm were compressed temporally by a factor of 5, to a duration of ~11 fs. The experimental results are supported by numerical simulations, showing that both Raman and Kerr effects play a role in the compression dynamics. The convenience of using ambient air, and the absence of glass windows that would distort the compressed pulses, makes the setup highly attractive as the basis of an efficien…
We present in detail our developed model [Saleh et al., Phys. Rev. Lett. 107] that governs pulse propagation in hollow-core photonic crystal fibers filled by an ionizing gas. By using perturbative methods, we find that the photoionization process induces the opposite phenomenon of the well-known Raman self-frequency red-shift of solitons in solid-core glass fibers, as was recently experimentally demonstrated [Hoelzer et al., Phys. Rev. Lett. 107]. This process is only limited by ionization losses, and leads to a constant acceleration of solitons in the time domain with a continuous blue-shift …
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…
We report on the experimental characterization of a novel nonlinear liquid-filled hollow-core photonic-crystal fiber for the generation of photon pairs at telecommunication wavelength through spontaneous four-wave-mixing. We show that the optimization procedure in view of this application links the choice of the nonlinear liquid to the design parameters of the fiber, and we give an example of such an optimization at telecom wavelengths. Combining the modeling of the fiber and classical characterization techniques at these wavelengths, we identify, for the chosen fiber and liquid combination, s…
Raman-scattering noise in silica has been the key obstacle toward the realisation of high quality fiber-based photon-pair sources. Here, we experimentally demonstrate how to get past this limitation by dispersion tailoring a xenon-filled hollow-core photonic crystal fiber. The source operates at room temperature, and is designed to generate Raman-free photon-pairs at useful wavelength ranges, with idler at the telecom, and signal at a visible range. We achieve a coincidence-to-accidentals ratio (2) as high as 2740 combined with an ultra low heralded g H (0) = 0.002, indicating a very high sign…
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…
An optical trapping scheme is proposed by which ultrashort low-amplitude radiations, co-propagating with a continuous train of temporal pulses in a hollow-core photonic crystal fiber filled with Raman-inactive noble gases, can be trapped and reshaped into optical soliton trains by means of cross-phase modulation interactions. The scheme complements and extends a recently proposed idea that a single-pulse soliton could trap an ultrashort small-amplitude radiation in a symmetric hollow-core photonic crystal fiber filled with a noble gas, thus preventing its dispersion [M. F. Saleh and F. Biancal…
The effective Kerr nonlinearity of hollow-core kagome-style photonic crystal fiber (PCF) filled with argon gas increases over 100 times when the pressure is increased from 1 to 150 bar, reaching 15 % of that of bulk silica glass, while the zero dispersion wavelength shifts from 300 to 900 nm. The group velocity dispersion of the system is uniquely pressure-tunable over a wide range while avoiding Raman scattering : absent in noble gases and having an extremely high optical damage threshold. As a result, detailed and well controlled studies of nonlinear effects can be performed, in both normal …
