We show that useful non-instantaneous nonlinear phase shifts can be obtained from cascaded quadratic processes in the presence of group velocity mismatch. The two-field nature of the process permits responses that can be effectively advanced or retarded in time with respect to one of the fields. There is an analogy to a generalized Raman-scattering effect, permitting both red and blue shifts of short pulses. We expect this capability to have many applications in short-pulse generation and propagation, such as the compensation of Raman-induced effects and high-quality pulse compression, which we discuss.
We introduce a new regime of cascaded quadratic nonlinearities which result in a continuous red shift of the optical pump, analogous to a Raman shifting process rather than self-phase modulation. This is particularly relevant to terahertz generation, where a continuous red shift of the pump can resolve current issues such as dispersion management and laser-induced damage. We show that in the absence of absorption or dispersion, the presented Raman shifting method will result in optical-to-terahertz energy conversion efficiencies that approach $100\%$ which is not possible with conventional cas…
Since the discovery of the laser, optical parametric nonlinearities have been at the core of efficient light conversion sources. Typically, thick transparent crystals or quasi-phase matched waveguides, are utilized in conjunction with phase-matching techniques to select a single parametric process. In recent years, due to the rapid developments in artificially structured materials, optical frequency mixing has been achieved at the nanoscale in subwavelength resonators arrayed as metasurfaces. Phase matching becomes relaxed for these wavelength-scale structures, and all allowed nonlinear proces…
We show that, in multimode Raman lasers, cascaded light scattering (CLS) not only extends the optical frequency range, but could also modulate the laser dynamics. The origin of this phenomenon is based on the fact that many Raman lasing modes are directly correlated through CLS. The coupled-mode equations only describe single-mode cascaded Raman lasers and are insufficient for describing the multimode case. In this work, we introduce additional terms to account for intermodal interaction and, thence, reveal the physical mechanism behind the mode-switching phenomenon. Additionally, mode-switchi…
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…
Due to their high circulating intensities, ultra-high quality factor dielectric whispering-gallery mode resonators have enabled the development of low threshold Raman microlasers. Subsequently, other Raman-related phenomena, such as cascaded stimulated Raman scattering (CSRS) and stimulated anti-Stokes Raman scattering (SARS), were observed. While low threshold frequency conversion and generation have clear applications, CSRS and SARS have been limited by the low Raman gain. In this work, the surface of a silica resonator is modified with an organic monolayer, increasing the Raman gain. Up to …
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…
Using system-reservoir methods to derive effective field theories for broadband nonlinear quantum optics: a case study on cascaded quadratic nonlinearities
We analyse Raman-induced self-frequency shift in two-component solitons supported by both quadratic and cubic nonlinearities. Treating Raman terms as a perturbation, we derive expressions for soliton velocity and frequency shifts of the fundamental frequency and second harmonic soliton components. We find these predictions compare well with simulations of soliton propagation. We also show that Raman shift can cause two-component solitons to approach the boundary of their own existence and subsequently trigger soliton instabilities. In some cases these instabilities are accompanied by an almost…
Molecular vibrations and their dynamics are of outstanding importance for electronic and thermal transport in nanoscale devices as well as for molecular catalysis. The vibrational dynamics of <100 molecules are studied through three-colour time-resolved coherent anti-Stokes Raman spectroscopy (trCARS) using plasmonic nanoantennas. This isolates molecular signals from four-wave mixing (FWM), while using exceptionally low nanowatt powers to avoid molecular damage via single-photon lock-in detection. FWM is found to be strongly suppressed in nm-wide plasmonic gaps compared to plasmonic nanopartic…
We report generation of cascaded rotational Raman scattering up to 58th orders in coherently excited CO_2 molecules. The high-order Raman scattering, which produces a quasiperiodic frequency comb with more than 600 sidebands, is obtained using an intense femtosecond laser to impulsively excite rotational coherence and the femtosecond-laser-induced N_2^+ lasing to generate cascaded Raman signals. The novel configuration allows this experiment to be performed with a single femtosecond laser beam at free-space standoff locations. It is revealed that the efficient spectral extension of Raman signa…
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…
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…
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. …
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…
In the numerical modelling of cascaded mid-infrared (IR) supercontinuum generation (SCG) we have studied how an ensemble of spectrally and temporally distributed solitons from the long-wavelength part of an SC evolves and interacts when coupled into the normal dispersion regime of a highly nonlinear chalcogenide fiber. This has revealed a novel fundamental phenomenon - the generation of a temporally and spectrally delocalized high energy rogue wave in the normal dispersion regime in the form of a strongly self-phase-modulation (SPM) broadened pulse. Along the local SPM shape the rogue wave is …
The recent advancement in lithium niobate on insulator (LNOI) technology is revolutionizing the optoelectronic industry as devices of higher performance, lower power consumption, and smaller footprint can be realized due to the high optical confinement in the structures. The LNOI platform offers both large \c{hi}(2) and \c{hi}(3) nonlinearities along with the power of dispersion engineering, enabling brand new nonlinear photonic devices and applications towards the next generation of integrated photonic circuits. However, the Raman scattering, one of the most important nonlinear phenomena, hav…
