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 highly nonlinear process. Numerical simulations based on a single broadband envelope equation with quadratic nonlinearity give estimates for the conversion efficiency within approximately 1 order of magnitude over a wide range of experimental parameters. From this comparison we identify a dimensionless parameter capturing the competition between three-wave mixing and group-velocity walk-off of the harmonics that governs the cascaded HHG physics. These results can inform cascaded HHG in a range of different platforms.
Frequency comb assisted diode laser spectroscopy, employing both the accuracy of an optical frequency comb and the broad wavelength tuning range of a tunable diode laser, has been widely used in many applications. In this letter we present a novel method using cascaded frequency agile diode lasers, which allows extending the measurement bandwidth to 37.4 THz (1355 to 1630 nm) at MHz resolution with scanning speeds above 1 THz/s. It is demonstrated as a useful tool to characterize a broadband spectrum for molecular spectroscopy and in particular it enables to characterize the dispersion of inte…
One of the essential goals of molecular spectroscopy is to measure all fundamental molecular vibrations simultaneously. To this end, one needs to measure broadband infrared (IR) absorption and Raman scattering spectra, which provide complementary vibrational information. A recently demonstrated technique called complementary vibrational spectroscopy (CVS) enables simultaneous measurements of IR and Raman spectra with a single device based on a single laser source. However, the spectral coverage was limited to ~1000 cm-1, which partially covers the spectral regions of the fundamental vibrations…
It is challenging for observing superbunching effect with true chaotic light, here we propose and demonstrate a method to achieve superbunching effect of the degree of second-order coherence is 2.42 with broadband stationary chaotic light based on a cascaded Michelson interferometer (CMI), exceeding the theoretical upper limit of 2 for the two-photon bunching effect of chaotic light. The superbunching correlation peak is measured with an ultrafast two-photon absorption detector which the full width at half maximum reaches about 95 fs. Two-photon superbunching theory in a CMI is developed to in…
Using system-reservoir methods to derive effective field theories for broadband nonlinear quantum optics: a case study on cascaded quadratic nonlinearities
The realization of ultrahigh quality (Q) resonators regardless of the underpinning material platforms has been a ceaseless pursuit, because the high Q resonators provide an extreme environment of storage of light to enable observations of many unconventional nonlinear optical phenomenon with high efficiencies. Here, we demonstrate an ultra-high Q factor (7.1*10^6) microresonator on the 4H-silicon-carbide-on-insulator (4H-SiCOI) platform in which both \c{hi}^(2) and \c{hi}^(3) nonlinear processes of high efficiencies have been generated. Broadband frequency conversions, including second-, third…
We study theoretically the cascaded four-wave mixing (FWM) in broadband tapered plasmonic nanoantennas and demonstrate a 300-fold increase in nonlinear frequency conversion detected in the main lobe of the nanoantenna far-field pattern. This is achieved by tuning the elements of the nanoantenna to resonate frequencies involved into the FWM interaction. Our findings have a potentially broad application in ultrafast nonlinear spectroscopy, sensing, on-chip optical frequency conversion, nonlinear optical metamaterials and photon sources.
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 report a broadband RF channelizer based on an integrated optical frequency Kerr micro-comb source, with an RF channelizing bandwidth of 90 GHz, a high RF spectral slice resolution of 1.04 GHz, and experimentally verify the RF performance up to 19 GHz. This approach to realizing RF channelizers offers reduced complexity, size, and potential cost for a wide range of applications to microwave signal detection.
For the growing demand of frequency combs in mid-infrared (mid-IR), known as the "molecular fingerprint" region of the spectrum [1], down conversion of near-IR frequency combs through half- harmonic generation offers numerous benefits including high conversion efficiency and intrinsic phase and frequency locking to the near-IR pump [2]. Hence cascaded half-harmonic generation promises a simple path towards extending the wavelength coverage of stable frequency combs. Here, we report a two-octave down-conversion of a frequency comb around 1 μm through cascaded half-harmonic generation with ~64% …
We introduce a new cascaded four-wave mixing technique which scales up the bandwidth of frequency combs generated by phase modulation of a continuous wave laser while simultaneously enhancing the spectral flatness. As a result we demonstrate a 10 GHz frequency comb with over 100 lines in a 10-dB bandwidth in which a record 75 lines are within a flatness of 1-dB. The cascaded four-wave mixing process increases the bandwidth of the initial comb generated by modulation of a CW laser by a factor of five. The broadband comb has approximately quadratic spectral phase, which is compensated upon propa…
Silicon nitride (Si$_3$N$_4$) is an ever-maturing integrated platform for nonlinear optics. Yet, due to the absence of second-order ($χ^{(2)}$) nonlinearity, Si$_3$N$_4$ is mostly considered for third-order ($χ^{(3)}$) nonlinear interactions. Recently, this limitation was overcome by optical poling in both Si$_3$N$_4$ waveguides and microresonators via the photogalvanic effect, resulting in the inscription of quasi-phase-matched $χ^{(2)}$ gratings. Here, we report cascaded nonlinear effects in a normal dispersion Si$_3$N$_4$ microresonator with combined $χ^{(2)}$ and $χ^{(3)}$ nonlinearities. …
We experimentally demonstrate a simple configuration for mid-infrared (MIR) frequency comb generation in quasi-phase-matched lithium niobate waveguides using the cascaded-$χ^{(2)}$ nonlinearity. With nanojoule-scale pulses from an Er:fiber laser, we observe octave-spanning supercontinuum in the near-infrared with dispersive-wave generation in the 2.5--3 $\textμ$m region and intra-pulse difference-frequency generation in the 4--5 $\textμ$m region. By engineering the quasi-phase-matched grating profiles, tunable, narrow-band MIR and broadband MIR spectra are both observed in this geometry. Final…
Breaking the reciprocity of light propagation in photonic integrated circuits (PIC) - especially in the CMOS-compatible silicon-on-insulator platform - is a topic of intense research. However, a practical solution for monolithic integrating of optical isolators and circulators remains elusive. Here, we propose and analyze a new non-reciprocal photonic architecture operating with standard single-mode waveguides (or optical fibers). Our design exploits cascaded phase modulators separated by optical delay lines and suitably driven by time shifted waveforms. Because it is based on fully balanced i…
Bright and broadband coherent mid-IR radiation is important for exciting and probing molecular vibrations. Using cascaded nonlinearities in conventional quadratic nonlinear crystal like lithium niobate, self-defocusing near-IR solitons have been demonstrated that led to very broadband supercontinuum generation in the visible, near-IR and short-wavelength mid-IR. Here we conduct an experiment where a mid-IR crystal pumped in the mid-IR gives multiple-octave spanning supercontinua. The crystal is cut for noncritical interaction, so the three-wave mixing of a single mid-IR femtosecond pump source…
We present an experimental study of optical frequency comb generation based on cascaded quadratic nonlinearities inside a continuous-wave-pumped optical parametric oscillator. We demonstrate comb states which produce narrow-linewidth intermode beat note signals, and we verify the mode spacing uniformity of the comb at the Hz level. We also show that spectral quality of the comb can be improved by modulating the parametric gain at a frequency that corresponds to the comb mode spacing. We have reached a high average output power of over 4 W in the near-infrared region, at ~2 μm.
Optical frequency comb generation by continuous-wave-pumped cascaded quadratic nonlinearities (CQN) appears a promising alternative to well-established modelocked lasers, especially if access to the mid-infrared spectral region is needed. We report an experimental investigation of spectral properties of a CQN frequency comb, which is based on second-harmonic generation (SHG) and is pumped internally by a continuous-wave optical parametric oscillator. Our study focuses on SHG phase mismatch, which has drawn little attention in the previously reported CQN frequency comb research. The main observ…
Optical frequency combs are revolutionising modern time and frequency metrology. In the past years, their range of applications has increased substantially, driven by their miniaturisation through microresonator-based solutions. The combs in such devices are typically generated using the third-order $χ^{(3)}$-nonlinearity of the resonator material. An alternative approach is making use of second-order $χ^{(2)}$-nonlinearities. While the idea of generating combs this way has been around for almost two decades, so far only few demonstrations are known, based either on bulky bow-tie cavities or o…
Superconducting nanowire single-photon detectors promise efficient (~100%) and fast (~Gcps) detection of light at the single-photon level. They constitute one of the building blocks to realize integrated quantum optical circuits in a waveguide architecture. The optical response of single-photon detectors, however, is limited to measure only the presence of photons. It misses the capability to resolve the spectrum of a possible broadband illumination. In this work, we propose the optical design for a superconducting nanowire single-photon spectrometer in an integrated optical platform. We explo…
We demonstrate a scheme, based on a cascade of lithium niobate intensity and phase modulators driven by specially tailored radio frequency waveforms to generate an optical frequency comb with very high spectral flatness. In this work we demonstrate a 10 GHz comb with ~40 lines with spectral power variation below 1-dB and ~60 lines in total. The number of lines that can be generated is limited by the power handling capability of the phase modulator, and this can be scaled without compromising the spectral flatness. Furthermore, the spectral phase of the generated combs in our scheme is almost p…
Cascaded stimulated Brillouin scattering (SBS) is a complex nonlinear optical process that results in the generation of several optical waves that are frequency shifted by an acoustic resonance frequency. Four-wave mixing (FWM) between these Brillouin shifted optical waves can create an equally spaced optical frequency comb with a stable spectral phase, i.e. a Brillouin frequency comb (BFC). Here, we investigate phase-locking of the spectral components of BFCs, considering FWM interactions arising from the Kerr-nonlinearity as well as from coupling by the acoustic field. Deriving for the first…
We present a novel approach to cascaded stimulated Brillouin scattering and frequency comb generation in which the multitude of interacting pump, Stokes, and anti-Stokes optical fields are described by a single forward wave and a single backward wave at a single carrier frequency. The envelopes of these two waves are modulated through coupling to a single acoustic oscillation and through four-wave mixing. Starting from a single pump field, we observe the emergence of a comb of frequencies as the intensity is increased. The set of three differential equations derived here are sufficient to desc…
We propose and analyze a new approach to generate a broadband astro-comb by spectral broadening of a narrowband astro-comb inside a highly nonlinear optical fiber. Numerical modeling shows that cascaded four-wave-mixing dramatically degrades the input comb's side-mode suppression and causes side-mode amplitude asymmetry. These two detrimental effects can systematically shift the center-of-gravity of astro-comb spectral lines as measured by an astrophysical spectrograph with resolution \approx100,000; and thus lead to wavelength calibration inaccuracy and instability. Our simulations indicate t…
We propose a new type of broadband and low repetition rate frequency comb generator which has the shape of an elongated and nanoscale-shallow optical bottle microresonator created at the surface of an optical fiber. The free spectral range (FSR) of the broadband azimuthal eigenfrequency series of this resonator is the exact multiple of the FSR of the dense and narrowband axial series. The effective radius variation of the microresonator is close to a parabola with a nanoscale height which is greater or equal to lambda/2pi*n0 (here lambda is the characteristic radiation wavelength and n0 is the…
Collective phenomena emerging from non-linear interactions between multiple oscillators, such as synchronization and frequency locking, find applications in a wide variety of fields. Optomechanical resonators, which are intrinsically non-linear, combine the scientific assets of mechanical devices with the possibility of long distance controlled interactions enabled by travelling light. Here we demonstrate light-mediated frequency locking of three distant nano-optomechanical oscillators positioned in a cascaded configuration. The oscillators, integrated on a chip along a coupling waveguide, are…
We present a monolithic solution to extract efficiently light from terahertz quantum cascade lasers with metal-metal waveguides suitable for broadband frequency comb applications. The design is optimized for a bandwidth of 500 GHz around a center frequency of 2.6 THz. A five-fold increase in total output power is observed compared to standard metal-metal waveguides. The extractor features a single-lobed far-field pattern and increases the frequency comb dynamical range to cover more than 50 % of the laser dynamic range. Frequency comb operation up to a spectral bandwidth of 670 GHz is achieved…
We demonstrate a novel approach to producing coherent, directional supercontinuum via cascaded dispersive wave generation. By pumping in the normal group-velocity dispersion regime, pulse compression of the first dispersive wave results in the generation of a second dispersive wave, resulting in an octave-spanning supercontinuum generated primarily to one side of the pump spectrum. We theoretically investigate the dynamics and show that the generated spectrum is highly coherent. We experimentally confirm this dynamical behavior and the coherence properties in silicon nitride waveguides by perf…
The outstanding phase-noise performance of optical frequency combs has led to a revolution in optical synthesis and metrology, covering a myriad of applications, from molecular spectroscopy to laser ranging and optical communications. However, the ideal characteristics of an optical frequency comb are application dependent. In this review, the different techniques for the generation and processing of high-repetition-rate (>10 GHz) optical frequency combs with technologies compatible with optical communication equipment are covered. Particular emphasis is put on the benefits and prospects of th…
Experimental data of femtosecond thick-crystal second-harmonic generation shows that when tuning away from phase matching, a dominating narrow spectral peak appears in the second harmonic that can be tuned over 100's of nm by changing the phase-mismatch parameter. Traditional theory explains this as phase matching between a sideband in the broadband pump to its second-harmonic. However, our experiment is conducted under high input intensities and instead shows excellent quantitative agreement with a nonlocal theory describing cascaded quadratic nonlinearities. This theory explains the detuned …
Two-photon excitation spectroscopy with broad spectral span is demonstrated at Doppler-limited resolution. We describe first Fourier transform two-photon spectroscopy of an atomic sample with two mode-locked laser oscillators in a dual-comb technique. Each transition is uniquely identified by the modulation imparted by the interfering comb excitations. The temporal modulation of the spontaneous two-photon fluorescence is monitored with a single photodetector, and the spectrum is revealed by a Fourier transform.
Historically, there has been a trade-off in spectroscopic measurements between high spectral resolution, broadband coverage, and acquisition time. Optical frequency combs, initially envisioned for precision spectroscopy of the hydrogen atom in the ultraviolet region, are now commonly used for probing molecular rotational-vibrational transitions throughout broad spectral bands in the mid-infrared with superior accuracy, resolution and speed. Here we demonstrate acquisition of 2.5 million spectral points over the continuous wavelength range of 3.2 to 5.1 microns (frequency span 1200 cm^{-1}, res…
We present detailed studies of the coherence properties of an ultra-broadband super-continuum, enabled by a new approach involving continuous wave laser sources to independently probe both the amplitude and phase noise quadratures across the entire spectrum. The continuum coherently spans more than 1.5 octaves, supporting Hz-level comparison of ultrastable lasers at 698 nm and 1.54 μm. We present the first numerical simulation of the accumulated comb coherence in the limit of many pulses, in contrast to the single-pulse level, with systematic experimental verification. The experiment and numer…
Development of chip-scale optical frequency comb with the coverage from ultra-violet (UV) to mid-infrared (MIR) wavelength is of great significance. To expand the comb spectrum into the challenging UV region, a material platform with high UV transparency is crucial. In this paper, crystalline aluminum nitride (AlN)-onsapphire film is demonstrated for efficient Kerr frequency comb generation. Near-infrared (NIR) comb with nearly octave-spanning coverage and low parametric threshold is achieved in continuous-wave pumped high-quality-factor AlN microring resonators. The competition between stimul…
We suggest a technique for using off-resonance spectral comb generation to produce broadband frequency modulated, and therefore, amplitude quieted light. Results include closed-form formulae for the amplitudes and phases of all of the spectral components.
We present homogeneous quantum cascade lasers (QCLs) emitting around 3 THz which display bandwidths up to 950 GHz with a single stable beatnote. Devices are spontaneously operating in a harmonic comb state, and when in a dense mode regime they can be injection locked at the cavity roundtrip frequency with very small RF powers down to -55 dBm. When operated in the electrically unstable region of negative differential resistance, the device displays ultra-broadband operation exceeding 1.83 THz ($Δf/f=50\%$) with high phase noise, exhibiting self-sustained, periodic voltage oscillations. The low …
We generate a 200-nm optical frequency comb at 1.5 microns by injecting two single-frequency lasers into a highly nonlinear fiber, and explore its spectral phase properties and high power to demonstrate full nonlinear conversion into its second harmonic. Combs of optical frequencies with 100-nm (~ 48 THz) bandwidths, centered at 790-800 nm and spaced by 0.8-1 nm (380-470 GHz) were produced by second harmonic and multiple sum frequency generation simply by focusing into a 2-mm long nonlinear crystal. Conventional birefringence phase matching was used in normal incidence configuration without ti…
We have recently introduced the Vernier-based Direct Frequency Comb Cavity-Enhanced Spectroscopy technique and we present the corresponding formalism for quantitative broadband spectroscopy. We achieve high sensitivity and broadband performance by acquiring spectra covering more than 2000 cm$^{-1}$ around 12600 cm$^{-1}$ (800 nm), resolving the 3$ν$+$δ$ band of water vapor and the entire A-band of oxygen in ambient air. 31 300 independent spectral elements are acquired at the second time scale with an absorption baseline noise of 2$\times$10$^{-8}$ cm$^{-1}$ providing a merit figure of 1,1.10$…
We demonstrate fiber mode-locked dual frequency comb spectroscopy for broadband, high resolution measurements in a rapid compression machine (RCM). We apply an apodization technique to improve the short-term signal-to-noise-ratio (SNR), which enables broadband spectroscopy at combustion-relevant timescales. We measure the absorption on 24345 individual wavelength elements (comb teeth) between 5967 and 6133 cm-1 at 704 microsecond time resolution during a 12-ms compression of a CH4-N2 mixture. We discuss the effect of the apodization technique on the absorption spectra, and apply an identical e…
Ultrasensitive detection of methane, isotopic carbon dioxide, carbon monoxide, formaldehyde, acetylene and ethylene is performed in the spectral range 2.5 - 5 μm using intracavity spectroscopy in broadband optical parametric oscillators (OPOs). The OPOs were operated near degeneracy and synchronously pumped either by a mode-locked erbium (1560 nm) or thulium (2050 nm) fiber laser. A large instantaneous bandwidth of up to 800 cm$^{-1}$ allows for simultaneous detection of several gases. We observe an effective path length enhancement due to coherent interaction inside the OPO cavity and achieve…
While being invented for precision measurement of single atomic transitions, frequency combs have also become a versatile tool for broadband spectroscopy in the last years. In this paper we present a novel and simple approach for broadband spectroscopy, combining the accuracy of an optical fiber-laser-based frequency comb with the ease-of-use of a tunable external cavity diode laser. This scheme enables broadband and fast spectroscopy of microresonator modes and allows for precise measurements of their dispersion, which is an important precondition for broadband optical frequency comb generati…
