The ultrafast optical Kerr effect (OKE) is widely used to investigate the structural dynamics and interactions of liquids, solutions and solids by observing their intrinsic nonlinear temporal responses through nearly-collinear four-wave mixing (FWM). Non-degenerate mixing schemes allow for background free detection and can provide information on the interplay between a material's internal degrees of freedom. Here we show a source of temporal dynamics in the OKE signal that is not reflective of the intrinsic nonlinear response but arises from group index and momentum mismatch. It is observed in two-color experiments on condensed media with sizable spectral dispersion, a common property near an optical resonance. In particular birefringence in crystalline solids is able to entirely change the character of the OKE signal via the off-diagonal tensor elements of the nonlinear susceptibility. We develop a detailed description of the phase-mismatched ultrafast OKE and show how to extract quantitative information on the spectrally resolved birefringence and group index from time-resolved experiments in one and two dimensions.
Dispersive Fourier transformation is a powerful technique in which the spectrum of an optical pulse is mapped into a time-domain waveform using chromatic dispersion. It replaces a diffraction grating and detector array with a dispersive fiber and single photodetector. This simplifies the system and, more importantly, enables fast real-time measurements. Here we describe a novel ultrafast barcode reader and displacement sensor that employs internally-amplified dispersive Fourier transformation. This technique amplifies and simultaneously maps the spectrally encoded barcode into a temporal wavef…
Taking advantage of an extended Lugiato--Lefever equation with third-order dispersion, we numerically show that dark cavity solitons formed in normal dispersion of microresonators are capable of emitting dispersive waves in both normal and anomalous dispersion regions, resembling the behavior of the commonly encountered bright cavity solitons. The generated dispersive waves can be accurately predicted by the dissipative radiation theory. In addition, we demonstrate the stability enhancement of Kerr frequency combs in normal dispersion regime in case the dispersive wave is emitted by dark solit…
It is critical to characterize the carrier and instantaneous frequency distribution variation in ultrafast processes, all of which are determined by the optical phase. Nevertheless, there is no method that can single-shot record the intro-pulse phase evolution of pico/femtosecond signals, to date. By analogying holographic principle in space to the time domain and using the time-stretch method, we propose the dispersive temporal holography to single-shot recover the phase and amplitude of ultrafast signals. It is a general and comprehensive technology and can be applied to analyze ultrafast si…
We performed non-degenerate pump-probe experiments on a GaAs/AlAs photonic structure. We switched the photonic properties using the optical Kerr effect and free carriers excited by three photon absorption. From these measurements we extracted the non-degenerate Kerr coefficients over a broad wavelength range and we extracted the three photon absorption coefficient for GaAs at three wavelengths in the near infrared. We show that the optical Kerr effect is large enough to switch a cavity resonance with a high \emph{Q} ($Q>1000$) photonic cavity.
We study the ultrafast Kerr effect and high-harmonic generation in type-II superconductors by formulating a new model for a time-varying electromagnetic pulse normally incident on a thin-film superconductor. It is found that type-II superconductors exhibit exceptionally large $χ^{(3)}$ due to the progressive destruction of Cooper pairs, and display high-harmonic generation at low incident intensities, and the highest nonlinear susceptibility of all known materials in the THz regime. Our theory opens up new avenues for accessible analytical and numerical studies of the ultrafast dynamics of sup…
Anomalous group velocity dispersion is a key parameter for generating bright solitons, and thus wideband Kerr frequency combs. Extension of frequency combs to visible wavelength in conventional photonic materials and structures has been a major challenge due to strong normal material dispersion at the relevant frequencies. Extension of frequency combs toward the normal dispersion region is possible via dispersive waves through soliton-induced Cherenkov radiation. However, this potentially powerful technique has not been used for extending frequency combs to the visible spectrum. In this paper,…
The ultrafast detection of single photons is currently restricted by the limited time resolution (a few picoseconds) of the available single-photon detectors. Optical gates offer a faster time resolution, but so far they have been mostly applied to ensembles of emitters. Here, we demonstrate through a semi-analytical model that the ultrafast time-resolved detection of single quantum emitters can be possible using an optical-Kerr-shutter (OKS) at GHz rates under focused illumination. This technique provides sub-picosecond time resolution, while keeping a gate efficiency at around 85 \%. These f…
Ultrashort pulses from Kerr-lens mode-locked oscillators have inspired a variety of applications. The design and alignment of these laser resonators have thus far been theoretically supported by the conventional analysis of beam propagation. However, the well-established theoretical framework is sometimes beyond the scope of high-peak-power oscillators. In this paper, we analyze the geometry of ring resonators by extending the ABCD-matrix method to a high-peak-power regime. The guidelines to achieving stable Kerr-lens mode-locking is provided for high-peak-power pulses.
A comprehensive experimental analysis of spatio-temporal coupling effects inherent to the acousto-optic programmable dispersive filter (AOPDF) is presented. Phase and amplitude measurements of the AOPDF transfer function are performed using spatially and spectrally resolved interferometry. Spatio-temporal and spatio-spectral coupling effects are presented for a range of shaped pulses that are commonly used in quantum control experiments. These effects are shown to be attributable to a single mechanism: a group-delay--dependent displacement of the shaped pulse. The physical mechanism is explain…
We introduce a mechanism to stabilize spatiotemporal solitons in Kerr nonlinear media, based on the dispersion of linear coupling between the field components forming the soliton states. Specifically, we consider solitons in a two-core guiding structure with inter-core coupling dispersion (CD). We show that CD profoundly affects properties of the solitons, causing the complete stabilization of the otherwise highly unstable spatiotemporal solitons in Kerr media with focusing nonlinearity. We also find that the presence of CD stimulates the formation of bound states, which however are unstable.
In this study we systematically measure the near-infrared spectral dependence, the sub-picosecond temporal evolution and pulse-width dependence of the effective Kerr coefficient ($n_{2,eff}$) of graphene in hundreds of femtosecond regime. The spectral dependence measured using the Z-scan technique is corroborated by quantum theory to extract a $n_{2,eff} \propto λ^2$ dependence. The temporal evolution extracted using the time-resolved Z-scan measurement shows the nonlinear response peaking at zero delay time and relaxing on a time scale of carrier relaxation. Since the Kerr-type response origi…
Ultrafast optical Kerr Gate at 1 GHz repetition rate by focusing on BBS glass
University of Siegen（锡根大学）；Alfred University（阿尔弗雷德大学）；European Laboratory for Non-Linear Spectroscopy（欧洲非线性光谱学实验室）；Università di Parma（帕尔马大学）；Istituto Nazionale di Ottica (INO), Consiglio Nazionale delle Ricerche (CNR)（意大利国家光学研究所，意大利国家研究委员会）
Imaging with ultrashort exposure times is generally achieved with a crossed-beam geometry. In the usual arrangement, an off-axis gating pulse induces birefringence in a medium exhibiting a strong Kerr response (commonly carbon disulfide) which is followed by a polarizer aligned to fully attenuate the on-axis imaging beam. By properly timing the gate pulse, imaging light experiences a polarization change allowing time-dependent transmission through the polarizer to form an ultrashort image. The crossed-beam system is effective in generating short gate times, however, signal transmission through…
Localized coherent structures can form in externally-driven dispersive optical cavities with a Kerr-type nonlinearity. Such systems are described by the Lugiato-Lefever equation, which supports a large variety of dynamical solutions. Here, we review our current knowledge on the formation, stability and bifurcation structure of localized structures in the one-dimensional Lugiato-Lefever equation. We do so by focusing on two main regimes of operation: anomalous and normal second-order dispersion. In the anomalous regime, localized patterns are organized in a homoclinic snaking scenario, which is…
We present a systematic study of ultrafast all-optical switching of Si photonic band gap woodpile crystals using broadband tunable nondegenerate pump-probe spectroscopy. At pump-probe coincidence, we investigate the behavior the differential reflectivity at the blue edge of the stopband for a wide range of pump- and probe frequencies. Both dispersive and absorptive features are observed from the probe spectra at coincidence. As the pump frequency is tuned through half the electronic bandgap of Si, the magnitude of both these features increases. For the first time we unambiguously identify this…
Dissipative Kerr solitons are self-sustaining optical wavepackets in resonators. They use the Kerr nonlinearity to both compensate dispersion and to offset optical loss. Besides providing insights into nonlinear resonator physics, they can be applied in frequency metrology, precision clocks, and spectroscopy. Like other optical solitons, the dissipative Kerr soliton can radiate power in the form of a dispersive wave through a process that is the optical analogue of Cherenkov radiation. Dispersive waves typically consist of an ensemble of optical modes. A limiting case is demonstrated in which …
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…
Quantum Dispersive Waves and Multimode Squeezing in Pure-Kerr Parametrically Driven Cavity Solitons
Institute for Physical Science and Technology, University of Maryland（马里兰大学物理科学与技术研究所）；Department of Physics, University of Maryland（马里兰大学物理系）；Department of Mechanical Engineering, University of Maryland（马里兰大学机械工程系）；University of Maryland Baltimore County（马里兰大学巴尔的摩县分校）；National Quantum Laboratory (QLab) at Maryland（马里兰国家量子实验室）
Plane waves in Kerr media spontaneously generate paraxial X-waves (i.e. non-dispersive and non-diffractive pulsed beams) that get amplified along propagation. This effect can be considered a form of conical emission (i.e. spatio-temporal modulational instability), and can be used as a key for the interpretation of the out of axis energy emission in the splitting process of focused pulses in normally dispersive materials. A new class of spatio-temporal localized wave patterns is identified. X-waves instability, and nonlinear X-waves, are also expected in periodical Bose condensed gases.
Temporal Kerr cavity solitons are pulses of light that can persist in coherently-driven, dispersive resonators with Kerr-type nonlinearity. It is widely accepted that such solitons react to parameter inhomogeneities by experiencing a temporal drift whose rate is governed by the gradient of the parameter at the soliton's position. This result, however, assumes that the gradient of the inhomogeneity is constant across the soliton, which may not hold true under all situations, e.g. when using bichromatic driving or in the presence of third-order dispersion that gives rise to an extended dispersiv…
We examine a coherently-driven, dispersion-managed, passive Kerr fiber ring resonator and report the first direct experimental observation of dispersive wave emission by temporal cavity solitons. Our observations are in excellent agreement with analytical predictions and they are fully corroborated by numerical simulations. These results lead to a better understanding of the behavior of temporal cavity solitons under conditions where higher-order dispersion plays a significant role. Significantly, since temporal cavity solitons manifest themselves in monolithic microresonators, our results are…
We present analytic threshold formulae applicable to both dispersive (time-domain) and diffractive (pattern-forming) instabilities in Fabry-Perot Kerr cavities of arbitrary finesse. We do so by extending the gain-circle technique, recently developed for counter-propagating fields in single-mirror-feedback systems, to allow for an input mirror. In time-domain counter-propagating systems walk-off effects are known to suppress cross-phase modulation contributions to dispersive instabilities. Applying the gain-circle approach with appropriately-adjusted cross-phase couplings extends previous resul…
Temporal cavity solitons (CSs) are pulses of light that can persist endlessly in dispersive, nonlinear optical resonators. They have been extensively studied in the context of resonators with purely cubic (Kerr-type) nonlinearity that are externally-driven with a monochromatic continuous wave laser -- in such systems, the solitons manifest themselves as unique attractors whose carrier frequency coincides with that of the external driving field. Recent experiments have, however, shown that a qualitatively different type of temporal CS can arise via parametric down-conversion in resonators with …
We demonstrate ultrafast all-optical deflection of spatial solitons in an AlGaAs slab waveguide using 190 fs, 1550 nm pulses which are used to generate and deflect the spatial soliton. The steering beam is focused onto the top of the waveguide near the soliton pathway and the soliton is steered due to refractive index changes induced by optical Kerr, or free carrier (Drude) effects. Angular deflections up to 8 mR are observed.
Carrier-envelope phase stabilization of optical pulses enables exquisitely precise measurements by way of direct optical-frequency synthesis, absolute optical-to-microwave phase conversion, and control of ultrafast waveforms. We report such phase stabilization for Kerr-microresonator frequency combs integrated on silicon chips, and verify their fractional-frequency inaccuracy at <3x10-16. Our work introduces an interlocked Kerr-comb configuration comprised of one silicon-nitride and one silica microresonator, which feature nearly harmonic repetition frequencies and can be generated with one la…
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…
The process of soliton Cherenkov radiation (also known as dispersive wave emission) in microresonator frequency combs plays a critical role in generating broadband and coherent microcomb spectra. Here, we report the observation of symmetry breaking in the group velocity of counter-propagating dissipative Kerr solitons, induced by polychromatic soliton Cherenkov radiation. Results show that in the presence of higher-order dispersion, the temporal arrangement of a multi-soliton state affects its group velocity, an effect which originates from the interference between multiple radiative tails emi…
We report on the comparative experimental investigation on third and fifth harmonic generation (THG and FHG) in atomic and molecular gases driven by mid-infrared ultrafast laser pulses at a wavelength of ~1500 nm. We observe that the conversion efficiencies of both the THG and FHG processes saturate at similar peak intensities close to ~1.5\times1014 W/cm2 for argon, nitrogen, and air, whose ionization potentials are close to each other. Near the saturation intensity, the ratio of yields of the FHG and THG reaches ~10-1 for all the gases. Our results show that high-order Kerr effects do exist,…
Università degli Studi di Salerno（萨莱诺大学）；CNR-SPIN, Unità di Salerno（意大利国家研究委员会自旋物理研究所萨莱诺分部）；CNISM, Unità di Salerno, Università degli Studi di Salerno（意大利纳米科学研究所萨莱诺分部，萨莱诺大学）
We present an optical Kerr effect based time-gate with the collinear incidence of the pump and probe beams at the Kerr medium, liquid carbon disulfide, for ballistic imaging of the high-pressure fuel sprays. The probe pulse used to illuminate the object under study is extracted from the supercontinuum generated by tightly focusing intense femtosecond laser pulses inside water, thereby destroying their coherence. The optical imaging spatial resolution and gate timings are investigated and compared with a similar setup without supercontinuum generation, where the probe is still coherent. And fin…
Precise measurement of multi-parameters of ultrafast lasers is vital both in scientific investigations and technical applications, such as, optical field manipulation, pulse shaping, sample characteristics test, and biomedical imaging. Tremendous progress in parameter measurement of ultrafast laser has been made, including single-shot spectra acquired by time-stretch dispersive Fourier transform in spectral domain, and pulse magnification or compression realized by time lens in temporal domain. Nevertheless, single-shot measurement of frequency-resolved states of polarization (SOPs) of ultrafa…
We present a complete and consistent quantum theory of generalised X waves with orbital angular momentum (OAM) in dispersive media. We show that the resulting quantised light pulses are affected by neither dispersion nor diffraction and are therefore resilient against external perturbations. The nonlinear interaction of quantised X waves in quadratic and Kerr nonlinear media is also presented and studied in detail.
Avoiding laser frequency drifts is a key issue in many atomic physics experiments. Several techniques have been developed to lock the laser frequency using sub-Doppler dispersive atomic lineshapes as error signals in a feedback loop. We propose here a two-beam technique that uses non-linear properties of an atomic vapor around sharp resonances to produce sub-Doppler dispersive-like lineshapes that can be used as error signals. Our simple and robust technique has the advantage of not needing either modulation or magnetic fields.
Recently an analytical model was presented that treats the nonlinear signal distortion from the Kerr nonlinearity in optical transmission systems as additive white Gaussian noise. This important model predicts the impact of the Kerr nonlinearity in systems operating at a high symbol rate and where the accumulated dispersion at the receiver is large. Starting from the suggested model for the propagating signal, we here give an independent and different calculation of the main result. The analysis is based on the Manakov equation with attenuation included and a complete and detailed derivation i…
Phonon-modulated Kerr nonlinearity in ultrathin 2H-MoTe2
Max Planck Institute for Solid State Research（马克斯·普朗克固体研究所）；Tsientang Institute for Advanced Study（紫江高等研究院）；Hefei National Laboratory, University of Science and Technology of China（合肥国家实验室，中国科学技术大学）；Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences（北京凝聚态物理国家实验室，中国科学院物理研究所）；School of Physical Sciences, University of Chinese Academy of Sciences（中国科学院大学物理科学学院）；Indian Institute of Science Education and Research（印度科学教育与研究机构）
A method is shown for preventing temporal broadening of ultrafast optical pulses in highly dispersive and fluctuating media for arbitrary signal-pulse profiles. Pulse pairs, consisting of a strong-field control-pulse and a weak-field signal-pulse co-propagate, whereby the specific profile of the strong-field pulse precisely compensates for dispersive phase in the weak pulse. A numerical example is presented in an optical system consisting of both resonant and gain dispersive effects. Here we show signal-pulses that do not temporally broaden across a vast propagation distance, even in the prese…
An ultrafast all-optical shutter is presented, based on a simple two-color two-photon absorption technique. For time-resolved luminescence measurements this shutter is an interesting alternative to the optical Kerr gate. The rejection efficiency is 99%, the switching-off and switching-on speeds are limited by the pulse length only, the rejection time is determined by the crystal slab thickness, and the bandwidth spans the entire visible spectrum. We show that our shutter can also be used for accurate measurement of group velocity inside a transparent material.
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…
Typically, strong gain saturation and gain dynamics play a crucial role in semiconductor laser mode-locking. While there have been several investigations of the ultrafast gain dynamics in vertical-external-cavity surface-emitting lasers (VECSELs), little is known about the associated refractive index changes. Yet, such refractive index changes do not only have a profound impact on the pulse formation process leading to self-phase modulation, which needs to be compensated by dispersion, but they are also of particular relevance for assessing the feasibility of Kerr-lens mode-locking of VECSELs.…
Dispersive shock waves (DSWs) are fascinating wave phenomena occurring in media when nonlinearity overwhelms dispersion (or diffraction). Creating DSWs with low generation power and realizing their active controls is desirable but remains a longstanding challenge. Here, we propose a scheme to generate weak-light DSWs and realize their manipulations in an atomic gas involving strongly interacting Rydberg states under the condition of electromagnetically induced transparency (EIT). We show that for a two-dimensional (2D) Rydberg gas a weak nonlocality of optical Kerr nonlinearity can significant…
We show that the extremely blue-shifted dispersive wave emitted in Kerr media owing to the coupling with the negative-frequency branch [Phys. Rev. Lett. {\bf 108}, 253901 (2012)] can be observed in quadratic media via second-harmonic generation. Not only such phenomenon is thus independent on the specific nonlinear mechanism, but it is shown to occur regardless of the fact that the process is pumped by a pulse which exhibits soliton-like features or, viceversa, undergoes wave-breaking. A simple unified formula gives the frequencies of the emitted dispersive waves in both cases.
Using the Kantorovitch method in combination with a Gaussian ansatz, we derive the equations of motion for spatial, temporal and spatiotemporal optical propagation in a dispersive Kerr medium with a general transverse and spectral gain profile. By rewriting the variational equations as differential equations for the temporal and spatial Gaussian q parameters, optical ABCD matrices for the Kerr effect, a general transverse gain profile and nonparabolic spectral gain filtering are obtained. Further effects can easily be taken into account by adding the corresponding ABCD matrices. Applications i…
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 …
In magnetoplasmonics, it is possible to tailor the magneto-optical properties of nanostructures by exciting surface plasmon polaritons (SPPs). Thus far, magnetoplasmonic effects have been considered static. Here, we describe ultrafast manifestations of magnetoplasmonics by observing the non-trivial evolution of the transverse magneto-optic Kerr effect within 45-fs pulses reflected from an iron-based magnetoplasmonic crystal. The effect occurs for resonant SPP excitations, displays opposite time derivative signs for different slopes of the resonance, and is explained with the magnetization-depe…
We study the anisotropic nature of the Kerr nonlinear response in a beta-barium borate (β-BaB2O4, BBO) nonlinear crystal. The focus is on determining the relevant $χ^{(3)}$ cubic tensor components that affect interaction of type I cascaded second-harmonic generation. Various experiments in the literature are analyzed and we correct the data from some of the experiments for contributions from cascading as well as for updated material parameters. We find that the Kerr nonlinear tensor component responsible for self-phase modulation in cascading is considerably larger than what has been used to d…
A novel setup is presented for ballistic imaging using an efficient ultrafast Kerr effect based optical time-gate with gating times of the order of ~0.8 picoseconds. At first, the major drawbacks of the classical non-collinear optical setup are discussed. Then, the new collinear arrangement is proposed, which overcomes these issues and improves the achievable imaging spatial resolution and gate timings. Few preliminary results for ballistic imaging of liquid sprays/jets are presented for this arrangement. It is shown that using a solid state Kerr medium (GGG crystal), instead of the classical …
