Iolanda Ricciardi

Frequency-comb-referenced singly-resonant OPO for sub-Doppler spectroscopy

We present a widely-tunable, singly-resonant optical parametric oscillator, emitting more than 1 W between 2.7 and 4.2 μm, which is phase locked to a self-referenced frequency comb. Both pump and signal frequencies are directly phase-locked to the frequency comb of a NIR-emitting fs mode-locked fibre laser, linked, in turn, to the caesium primary standard. We estimate for the idler frequency a fractional Allan deviation of ∼ 3 × 10⁻¹²τ⁻½ between 1 and 200 s. To test the spectroscopic performance of the OPO, we carried out saturation spectroscopy of several transitions belonging to the ν1 rovibrational band of CH₃I, resolving their electronic quadrupole hyperfine structure, estimating a linewidth better than 200 kHz FWHM for the idler, and determining the absolute frequency of the hyperfine components with a 50-kHz-uncertainty.

Frequency comb generation in quadratic nonlinear media

We experimentally demonstrate and theoretically explain the onset of optical frequency combs in a simple cavity-enhanced second-harmonic-generation system, exploiting second-order nonlinear interactions. Two combs are simultaneously generated around the fundamental pump frequency, with a spectral bandwidth up to about 10 nm, and its second harmonic. We observe different regimes of generation, depending on the phase-matching condition for second-harmonic-generation. Moreover, we develop an elemental model which provides a deep physical insight into the observed dynamics. Despite the different underlying physical mechanism, the proposed model is remarkably similar to the description of third-order effects in microresonators, revealing a potential variety of new effects to be explored and laying the groundwork for a novel class of highly efficient and versatile frequency comb synthesizers based on second-order nonlinear materials.

Walk-Off-Induced Modulation Instability, Temporal Pattern Formation, and Frequency Comb Generation in Cavity-Enhanced Second-Harmonic Generation.

We derive a time-domain mean-field equation to model the full temporal and spectral dynamics of light in singly resonant cavity-enhanced second-harmonic generation systems. We show that the temporal walk-off between the fundamental and the second-harmonic fields plays a decisive role under realistic conditions, giving rise to rich, previously unidentified nonlinear behavior. Through linear stability analysis and numerical simulations, we discover a new kind of quadratic modulation instability which leads to the formation of optical frequency combs and associated time-domain dissipative structures. Our numerical simulations show excellent agreement with recent experimental observations of frequency combs in quadratic nonlinear media [Phys. Rev. A 91, 063839 (2015)]. Thus, in addition to unveiling a new, experimentally accessible regime of nonlinear dynamics, our work enables predictive modeling of frequency comb generation in cavity-enhanced second-harmonic generation systems. We expect our findings to have wide impact on the study of temporal and spectral dynamics in a diverse range of dispersive, quadratically nonlinear resonators.

Sum-frequency generation of cw ultraviolet radiation in periodically poled LiTaO(3).

We present cw sum-frequency generation of UV radiation at 355 nm based on a high-power laser at 1064 nm and a two-stage quasi-phase-matching nonlinear interaction in periodically poled LiTaO3 crystals. In a first stage, second harmonic at 532 nm is generated. Then, the outcoming IR and green light interact in a second nonlinear crystal to generate about 7 mW of ultraviolet radiation at the sum frequency.

Frequency comb formation in doubly resonant second-harmonic generation

We theoretically study the generation of optical frequency combs and corresponding pulse trains in doubly resonant intracavity second-harmonic generation (SHG). We find that, despite the large temporal walk-off characteristic of realistic cavity systems, the nonlinear dynamics can be accurately and efficiently modeled using a pair of coupled mean-field equations. Through rigorous stability analysis of the systems steady-state continuous-wave solutions, we demonstrate that walk-off can give rise to an unexplored regime of temporal modulation instability. Numerical simulations performed in this regime reveal rich dynamical behaviors, including the emergence of temporal patterns that correspond to coherent optical frequency combs. We also demonstrate that the two coupled equations that govern the doubly resonant cavity behavior can, under typical conditions, be reduced to a single mean-field equation akin to that describing the dynamics of singly-resonant-cavity SHG [F. Leo et al., Phys. Rev. Lett. 116, 033901 (2016)]. This reduced approach allows us to derive a simple expression for the modulation instability gain, thus permitting us to acquire significant insight into the underlying physics. We anticipate that our work will have a wide impact on the study of frequency combs in emerging doubly resonant cavity SHG platforms, including quadratically nonlinear microresonators.

Single envelope equation modeling of multi-octave comb arrays in microresonators with quadratic and cubic nonlinearities

We numerically study, by means of the single envelope equation, the generation of optical frequency combs ranging from the visible to the mid-infrared spectral regions in resonators with quadratic and cubic nonlinearities. Phase-matched quadratic wave-mixing processes among the comb lines can be activated by low-power continuous wave pumping in the near infrared of a radially poled lithium niobate whispering gallery resonator. We examine both separate and coexisting intracavity doubly resonant second-harmonic generation and parametric oscillation processes and find that modulation instabilities may lead to the formation of coupled comb arrays extending over multiple octaves. In the temporal domain, the frequency combs may correspond to pulse trains or even to a single pulse circulating in the cavity.

SPECIAL issue: 22nd colloquium on high-resolution molecular spectroscopy HRMS Dijon 2011 (Part 2) A narrow-linewidth optical parametric oscillator for mid-infrared high-resolution spectroscopy

We present a narrow-linewidth, singly-resonant cw optical parametric oscillator, emitting more than 1 W in the 2.7–4.2 µm range. The OPO is pumped by a narrow linewidth (40 kHz) fibre-laser system and the signal frequency is locked to a high-finesse Fabry–Pérot cavity in order to increase the spectral resolution, thus obtaining a residual linewidth of 70 kHz for the signal. We tested the spectral performance of our OPO on several transitions in the ν1 rovibrational band of CH3I, measuring line intensities and showing sub-Doppler dip detection.

High-speed multi-THz-range mode-hop-free tunable mid-IR laser spectrometer.

We report on a widely (2.25 THz or 75 cm(-1)) and rapidly (4.5 THz/s) mode-hop-free (MHF) tunable mid-IR laser source at ~3.3 μm, consisting of a 5%-MgO:LiNbO(3) singly resonant optical parametric oscillator (SRO) pumped by an automated broadly MHF tunable extended-cavity diode laser (ECDL). The broad and rapid MHF tuning capability of the ECDL is readily transferred to the SRO idler wave owing to the quasi-noncritical pump spectral acceptance bandwidth of the quasi-phase-matching. Fast and broadband high-resolution Doppler spectroscopy measurements of the ν(3) band of CH(4) are presented to illustrate the performance of the mid-IR optical parametric oscillator spectrometer.

Cavity-enhanced generation of 6 W cw second-harmonic power at 532 nm in periodically-poled MgO:LiTaO 3

We report on efficient cw high-power second harmonic generation in a periodically poled LiTaO3 crystal placed in a resonant enhancement cavity. We tested three configurations, differing in the coupling mirror reflectivity, and a maximum conversion efficiency of about 76%, corresponding to 6.1 W of green light with 8.0 W of fundamental power, was achieved. This is, to the best of our knowledge, the highest cw power ever reported using a periodically-poled crystal in an external cavity. We observed photo-thermal effect induced by photon absorption at the mirrors and in the crystal, which however does not affect stable operation of the cavity. A further effect arises for two out of the three configurations, at higher values of the input power, which degrades the performance of the locked cavity. We suggest this effect is due to the onset of competing nonlinearities in the same crystal.

Direct generation of optical frequency combs in χ(2) nonlinear cavities

Abstract Quadratic nonlinear processes are currently exploited for frequency comb transfer and extension from the visible and near infrared regions to other spectral ranges where direct comb generation cannot be accomplished. However, frequency comb generation has been directly observed in continuously pumped quadratic nonlinear crystals placed inside an optical cavity. At the same time, an introductory theoretical description of the phenomenon has been provided, showing a remarkable analogy with the dynamics of third-order Kerr microresonators. Here, we give an overview of our recent work on χ(2) frequency comb generation. Furthermore, we generalize the preliminary three-wave spectral model to a many-mode comb and present a stability analysis of different cavity field regimes. Although our work is a very early stage, it lays the groundwork for a novel class of highly efficient and versatile frequency comb synthesizers based on second-order nonlinear materials.