Observation of quantum-correlated twin beams in cascaded nonlinear interactions.

We report on the generation of twin beams through a cascaded process of optical parametric oscillation in a doubly resonant second-harmonic generation system. These bright beams exhibit strong quantum correlations, enabling the observation of up to 5 dB of noise reduction in their intensity difference below the standard quantum limit.

Optical frequency combs in dispersion-controlled doubly resonant second-harmonic generation.

We report on the experimental realization and a systematic study of optical frequency comb generation in doubly resonant intracavity second harmonic generation (SHG). The efficiency of intracavity nonlinear processes usually benefits from the increasing number of resonating fields. Yet, achieving the simultaneous resonance of different fields may be technically complicated, all the more when a phase matching condition must be fulfilled as well. In our cavity we can separately control the resonance condition for the fundamental and its second harmonic, by simultaneously acting on an intracavity dispersive element and on a piezo-mounted cavity mirror, without affecting the quasi-phase matching condition. In addition, by finely adjusting the laser-to-cavity detuning, we are able to observe steady comb emission across the whole resonance profile, revealing the multiplicity of comb structures, and the substantial role of thermal effects on their dynamics. Lastly, we report the results of numerical simulations of comb dynamics, which include photothermal effects, finding a good agreement with the experimental observations. Our system provides a framework for exploring the richness of comb dynamics in doubly resonant SHG systems, assisting the design of chip-scale quadratic comb generators.

Absolute frequency stabilization of a QCL at 8.6 µm by modulation transfer spectroscopy.

Modulation transfer spectroscopy is used to demonstrate absolute frequency stabilization of an 8.6-µm-wavelength quantum cascade laser against a sub-Doppler absorption of the CHF3 molecule. The obtained spectral emission properties are thoroughly characterized through a self-referenced optical frequency comb, stabilized against either a GPS-disciplined Rb clock or a 1.54-µm Er-fiber laser locked to a high-finesse ultra-low-expansion optical cavity. Fractional long-term stability and accuracy at a level of 4×10-12 (at 100 s) and 3×10-10, respectively, are demonstrated, along with an emission linewidth as narrow as 10 kHz for observation times of 0.1 s.

Infrared Comb Spectroscopy of Buffer-Gas-Cooled Molecules: Toward Absolute Frequency Metrology of Cold Acetylene.

We review the recent developments in precision ro-vibrational spectroscopy of buffer-gas-cooled neutral molecules, obtained using infrared frequency combs either as direct probe sources or as ultra-accurate optical rulers. In particular, we show how coherent broadband spectroscopy of complex molecules especially benefits from drastic simplification of the spectra brought about by cooling of internal temperatures. Moreover, cooling the translational motion allows longer light-molecule interaction times and hence reduced transit-time broadening effects, crucial for high-precision spectroscopy on simple molecules. In this respect, we report on the progress of absolute frequency metrology experiments with buffer-gas-cooled molecules, focusing on the advanced technologies that led to record measurements with acetylene. Finally, we briefly discuss the prospects for further improving the ultimate accuracy of the spectroscopic frequency measurement.

Absolute frequency measurements of CHF3 Doppler-free ro-vibrational transitions at 8.6 µm.

We report on absolute measurements of saturated-absorption line-center frequencies of room-temperature trifluoromethane using a quantum cascade laser at 8.6 µm and the frequency modulation spectroscopy method. Absolute calibration of the laser frequency is obtained by direct comparison with a mid-infrared optical frequency comb synthesizer referenced to a radio-frequency Rb standard. Several sub-Doppler transitions falling in the υ5 vibrational band are investigated at around 1158.9 cm-1 with a fractional frequency precision of 8.6·10-12 at 1-s integration time, limited by the Rb-clock stability. The demonstrated frequency uncertainty of 6.6·10-11 is mainly limited by the reproducibility of the frequency measurements.

Comb-assisted cavity ring-down spectroscopy of a buffer-gas-cooled molecular beam.

We demonstrate continuous-wave cavity ring-down spectroscopy of a partially hydrodynamic molecular beam emerging from a buffer-gas-cooling source. Specifically, the (ν1 + ν3) vibrational overtone band of acetylene (C2H2) around 1.5 µm is accessed using a narrow-linewidth diode laser stabilized against a GPS-disciplined rubidium clock via an optical frequency comb synthesizer. As an example, the absolute frequency of the R(1) component is measured with a fractional accuracy of ∼1 × 10(-9). Our approach represents the first step towards the extension of more sophisticated cavity-enhanced interrogation schemes, including saturated absorption cavity ring-down or two-photon excitation, to buffer-gas-cooled molecular beams.

Frequency-comb-assisted precision laser spectroscopy of CHF3 around 8.6 µm.

We report a high-precision spectroscopic study of room-temperature trifluoromethane around 8.6 µm, using a CW quantum cascade laser phase-locked to a mid-infrared optical frequency comb. This latter is generated by a nonlinear down-conversion process starting from a dual-branch Er:fiber laser and is stabilized against a GPS-disciplined rubidium clock. By tuning the comb repetition frequency, several transitions falling in the υ5 vibrational band are recorded with a frequency resolution of 20 kHz. Due to the very dense spectra, a special multiple-line fitting code, involving a Voigt profile, is developed for data analysis. The combination of the adopted experimental approach and survey procedure leads to fractional accuracy levels in the determination of line center frequencies, down to 2 × 10(-10). Line intensity factors, pressure broadening, and shifting parameters are also provided.

Phase noise analysis of a 10 Watt Yb-doped fibre amplifier seeded by a 1-Hz-linewidth laser.

We report a thorough analysis of the spectral properties of an ytterbium-doped fibre amplifier, seeded by a Nd:YAG laser, whose linewidth has been narrowed down to 1 Hz by locking the laser to an ultrastable reference cavity. We measured the phase noise contribution from the amplifier, showing that it does not depend on the amplification gain, nor on the seed laser linewidth. Moreover, the amplifier-induced phase noise does not affect the final linewidth, as verified by heterodyne linewidth measurement within the 0.2 Hz resolution bandwidth of our acquisition set-up. Preservation of spectral purity below Hz-level is promising for more demanding applications, from nonlinear optics to frequency/time-standard transfer over fibre links.

Absolute frequency metrology of buffer-gas-cooled molecular spectra at 1 kHz accuracy level.

By reducing both the internal and translational temperature of any species down to a few kelvins, the buffer-gas-cooling (BGC) technique has the potential to dramatically improve the quality of ro-vibrational molecular spectra, thus offering unique opportunities for transition frequency measurements with unprecedented accuracy. However, the difficulty in integrating metrological-grade spectroscopic tools into bulky cryogenic equipment has hitherto prevented from approaching the kHz level even in the best cases. Here, we overcome this drawback by an original opto-mechanical scheme which, effectively coupling a Lamb-dip saturated-absorption cavity ring-down spectrometer to a BGC source, allows us to determine the absolute frequency of the acetylene (ν1 + ν3) R(1)e transition at 6561.0941 cm-1 with a fractional uncertainty as low as 6 × 10-12. By improving the previous record with buffer-gas-cooled molecules by one order of magnitude, our approach paves the way for a number of ultra-precise low-temperature spectroscopic studies, aimed at both fundamental Physics tests and optimized laser cooling strategies.

Optical Frequency Combs in Quadratically Nonlinear Resonators.

Optical frequency combs are one of the most remarkable inventions in recent decades. Originally conceived as the spectral counterpart of the train of short pulses emitted by mode-locked lasers, frequency combs have also been subsequently generated in continuously pumped microresonators, through third-order parametric processes. Quite recently, direct generation of optical frequency combs has been demonstrated in continuous-wave laser-pumped optical resonators with a second-order nonlinear medium inside. Here, we present a concise introduction to such quadratic combs and the physical mechanism that underlies their formation. We mainly review our recent experimental and theoretical work on formation and dynamics of quadratic frequency combs. We experimentally demonstrated comb generation in two configurations: a cavity for second harmonic generation, where combs are generated both around the pump frequency and its second harmonic and a degenerate optical parametric oscillator, where combs are generated around the pump frequency and its subharmonic. The experiments have been supported by a thorough theoretical analysis, aimed at modelling the dynamics of quadratic combs, both in frequency and time domains, providing useful insights into the physics of this new class of optical frequency comb synthesizers. Quadratic combs establish a new class of efficient frequency comb synthesizers, with unique features, which could enable straightforward access to new spectral regions and stimulate novel applications.

Axion dark matter detection by laser induced fluorescence in rare-earth doped materials.

We present a detection scheme to search for QCD axion dark matter, that is based on a direct interaction between axions and electrons explicitly predicted by DFSZ axion models. The local axion dark matter field shall drive transitions between Zeeman-split atomic levels separated by the axion rest mass energy m a c 2. Axion-related excitations are then detected with an upconversion scheme involving a pump laser that converts the absorbed axion energy (~hundreds of µeV) to visible or infrared photons, where single photon detection is an established technique. The proposed scheme involves rare-earth ions doped into solid-state crystalline materials, and the optical transitions take place between energy levels of 4f N electron configuration. Beyond discussing theoretical aspects and requirements to achieve a cosmologically relevant sensitivity, especially in terms of spectroscopic material properties, we experimentally investigate backgrounds due to the pump laser at temperatures in the range 1.9 - 4.2 K. Our results rule out excitation of the upper Zeeman component of the ground state by laser-related heating effects, and are of some help in optimizing activated material parameters to suppress the multiphonon-assisted Stokes fluorescence.