Precise radiocarbon determination in radioactive waste by a laser-based spectroscopic technique.

The precise and accurate determination of the radionuclide inventory in radioactive waste streams, including those generated during nuclear decommissioning, is a key aspect in establishing the best-suited nuclear waste management and disposal options. Radiocarbon ([Formula: see text]) is playing a crucial role in this scenario because it is one of the so-called difficult to measure isotopes; currently, [Formula: see text] analysis requires complex systems, such as accelerator mass spectrometry (AMS) or liquid scintillation counting (LSC). AMS has an outstanding limit of detection, but only a few facilities are available worldwide; LSC, which can have similar performance, is more widespread, but sample preparation can be nontrivial. In this paper, we demonstrate that the laser-based saturated-absorption cavity ring-down (SCAR) spectroscopic technique has several distinct advantages and represents a mature and accurate alternative for [Formula: see text] content determination in nuclear waste. As a proof-of-principle experiment, we show consistent results of AMS and SCAR for samples of concrete and graphite originating from nuclear installations. In particular, we determined mole fractions of 1.312(9) F[Formula: see text] and 30.951(7) F[Formula: see text] corresponding to ∼1.5 and 36.2 parts per trillion (ppt), respectively, for two different graphite samples originating from different regions of the Adiabatic Resonance Crossing activator prototype installed on one irradiation line of an MC40 Scanditronix cyclotron. Moreover, we measure a mole fraction of 0.593(8) F[Formula: see text] ([Formula: see text] ppt) from a concrete sample originating from an external wall of the Ispra-1 nuclear research reactor currently in the decommissioning phase.

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.

Fiber-optic gyroscope for rotational seismic ground motion monitoring of the Campi Flegrei volcanic area.

The real-time monitoring of densely populated areas with high seismic and volcanic risk is of crucial importance for the safety of people and infrastructures. When an earthquake occurs, the Earth surface experiences both translational and rotational motions. The latter are usually not monitored, but their measurement and characterization are essential for a full description of the ground motion. Here we present preliminary observational data of a high-sensitivity rotational sensor based on a 2-km-long fiber-optic Sagnac gyroscope, presently under construction in the middle of the Campi Flegrei Volcanic Area (Pozzuoli, Italy). We have evaluated its performance by analyzing data continuously recorded during an acquisition campaign of five months. The experimental setup was composed of a digital nine-component seismic station equipped with both a rotational sensor and conventional seismic sensors (seismometers, accelerometers, and tiltmeters). During this experiment we detected seismic noise and ground rotations wavefield induced by small to medium local earthquakes (M D<3). The prototype gyroscope shows a very promising sensitivity in the range of 5×10-7-8×10-9 r a d/s/H z over the frequency bandwidth 5 mHz-50 Hz. Future upgrades and perspectives are discussed.

Time/frequency-domain characterization of a mid-IR DFG frequency comb via two-photon and heterodyne detection.

Mid-infrared frequency combs are nowadays well-appreciated sources for spectroscopy and frequency metrology. Here, a comprehensive approach for characterizing a difference-frequency-generated mid-infrared frequency comb (DFG-comb) both in the time and in the frequency domain is presented. An autocorrelation scheme exploiting mid-infrared two-photon detection is used for characterizing the pulse width and to verify the optimal compression of the generated pulses reaching a pulse duration (FWHM) as low as 196 fs. A second scheme based on mid-infrared heterodyne detection employing two independent narrow-linewidth quantum cascade lasers (QCLs) is used for frequency-narrowing the modes of the DFG-comb down to 9.4 kHz on a 5-ms timescale.

Analog FM free-space optical communication based on a mid-infrared quantum cascade laser frequency comb.

Quantum cascade laser frequency combs are nowadays well-appreciated sources for infrared spectroscopy. Here their applicability for free-space optical communication is demonstrated. The spontaneously-generated intermodal beat note of the frequency comb is used as carrier for transferring the analog signal via frequency modulation. Exploiting the atmospheric transparency window at 4 µm, an optical communication with a signal-to-noise ratio up to 65 dB is realized, with a modulation bandwidth of 300 kHz. The system tolerates a maximum optical attenuation exceeding 35 dB. The possibility of parallel transmission of an independent digital signal via amplitude modulation at 5 Mbit/s is also demonstrated.

Characterization of noise regimes in mid-IR free-space optical communication based on quantum cascade lasers.

The recent development of Quantum Cascade Lasers (QCLs) represents one of the biggest opportunities for the deployment of a new class of Free Space Optical (FSO) communication systems working in the mid-infrared (mid-IR) wavelength range. As compared to more common FSO systems exploiting the telecom range, the larger wavelength employed in mid-IR systems delivers exceptional benefits in case of adverse atmospheric conditions, as the reduced scattering rate strongly suppresses detrimental effects on the FSO link length given by the presence of rain, dust, fog, and haze. In this work, we use a novel FSO testbed operating at 4.7 µm, to provide a detailed experimental analysis of noise regimes that could occur in realistic FSO mid-IR systems based on QCLs. Our analysis reveals the existence of two distinct noise regions, corresponding to different realistic channel attenuation conditions, which are precisely controlled in our setup. To relate our results with real outdoor configurations, we combine experimental data with predictions of an atmospheric channel loss model, finding that error-free communication could be attained for effective distances up to 8 km in low visibility conditions of 1 km. Our analysis of noise regimes may have a key relevance for the development of novel, long-range FSO communication systems based on mid-IR QCL sources.

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.

Mid-infrared homodyne balanced detector for quantum light characterization.

We present the characterization of a novel balanced homodyne detector operating in the mid-infrared. The challenging task of revealing non-classicality in mid-infrared light, e. g. in quantum cascade lasers emission, requires a high-performance detection system. Through the intensity noise power spectral density analysis of the differential signal coming from the incident radiation, we show that our setup is shot-noise limited. We discuss the experimental results with a view to possible applications to quantum technologies, such as free-space quantum communication.

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.

Liquid Droplet Microresonators.

We provide here an overview of passive optical micro-cavities made of droplets in the liquid phase. We focus on resonators that are naturally created and suspended under gravity thanks to interfacial forces, illustrating simple ways to excite whispering-gallery modes in various slow-evaporation liquids using free-space optics. Similar to solid resonators, frequency locking of near-infrared and visible lasers to resonant modes is performed exploiting either phase-sensitive detection of the leakage cavity field or multiple interference between whispering-gallery modes in the scattered light. As opposed to conventional micro-cavity sensors, each droplet acts simultaneously as the sensor and the sample, whereby the internal light can detect dissolved compounds and particles. Optical quality factors up to 107⁻108 are observed in liquid-polymer droplets through photon lifetime measurements. First attempts in using single water droplets are also reported. These achievements point out their huge potential for direct spectroscopy and bio-chemical sensing in liquid environments. Finally, the first experiments of cavity optomechanics with surface acoustic waves in nanolitre droplets are presented. The possibility to perform studies of viscous-elastic properties points to a new paradigm: a droplet device as an opto-fluid-mechanics laboratory on table-top scale under controlled environmental conditions.

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.

Tunable Microcavity-Stabilized Quantum Cascade Laser for Mid-IR High-Resolution Spectroscopy and Sensing.

The need for highly performing and stable methods for mid-IR molecular sensing and metrology pushes towards the development of more and more compact and robust systems. Among the innovative solutions aimed at answering the need for stable mid-IR references are crystalline microresonators, which have recently shown excellent capabilities for frequency stabilization and linewidth narrowing of quantum cascade lasers with compact setups. In this work, we report on the first system for mid-IR high-resolution spectroscopy based on a quantum cascade laser locked to a CaF2 microresonator. Electronic locking narrows the laser linewidth by one order of magnitude and guarantees good stability over long timescales, allowing, at the same time, an easy way for finely tuning the laser frequency over the molecular absorption line. Improvements in terms of resolution and frequency stability of the source are demonstrated by direct sub-Doppler recording of a molecular line.

Quantum cascade lasers: 20 years of challenges.

We review the most recent technological and application advances of quantum cascade lasers, underlining the present milestones and future directions from the Mid-infrared to the Terahertz spectral range. Challenges and developments, which are the subject of the contributions to this focus issue, are also introduced.

High finesse optical cavity coupled with a quartz-enhanced photoacoustic spectroscopic sensor.

An ultra-sensitive and selective quartz-enhanced photoacoustic spectroscopy (QEPAS) combined with a high-finesse cavity sensor platform is proposed as a novel method for trace gas sensing. We call this technique Intra-cavity QEPAS (I-QEPAS). In the proposed scheme, a single-mode continuous wave quantum cascade laser (QCL) is coupled into a bow-tie optical cavity. The cavity is locked to the QCL emission frequency by means of a feedback-locking loop that acts directly on a piezoelectric actuator mounted behind one of the cavity mirrors. A power enhancement factor of ∼240 was achieved, corresponding to an intracavity power of ∼0.72 W. CO2 was selected as the target gas to validate our sensor. For the P(42) CO2 absorption line, located at 2311.105 cm(-1), a minimum detection limit of 300 parts per trillion by volume at a total gas pressure of 50 mbar was achieved with a 20 s integration time. This corresponds to a normalized noise equivalent absorption of 3.2 × 10(-10) W cm(-1) Hz(-1/2), comparable with the best results reported for the QEPAS technique on much faster relaxing gases. A comparison with standard QEPAS performed under the same experimental conditions confirms that the I-QEPAS sensitivity scales with the intracavity laser power enhancement factor.

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.

Ionizing radiation detectors based on Ge-doped optical fibers inserted in resonant cavities.

The measurement of ionizing radiation (IR) is a crucial issue in different areas of interest, from environmental safety and industrial monitoring to aerospace and medicine. Optical fiber sensors have recently proven good candidates as radiation dosimeters. Here we investigate the effect of IR on germanosilicate optical fibers. A piece of Ge-doped fiber enclosed between two fiber Bragg gratings (FBGs) is irradiated with gamma radiation generated by a 6 MV medical linear accelerator. With respect to other FBG-based IR dosimeters, here the sensor is only the bare fiber without any special internal structure. A near infrared laser is frequency locked to the cavity modes for high resolution measurement of radiation induced effects on the fiber optical parameters. In particular, we observe a variation of the fiber thermo-optic response with the radiation dose delivered, as expected from the interaction with Ge defect centers, and demonstrate a detection limit of 360 mGy. This method can have an impact in those contexts where low radiation doses have to be measured both in small volumes or over large areas, such as radiation therapy and radiation protection, while bare optical fibers are cheap and disposable.

Cavity-enhanced photoacoustic dual-comb spectroscopy.

Photoacoustic dual-comb spectroscopy (DCS), converting spectral information in the optical frequency domain to the audio frequency domain via multi-heterodyne beating, enables background-free spectral measurements with high resolution and broad bandwidth. However, the detection sensitivity remains limited due to the low power of individual comb lines and the lack of broadband acoustic resonators. Here, we develop cavity-enhanced photoacoustic DCS, which overcomes these limitations by using a high-finesse optical cavity for the power amplification of dual-frequency combs and a broadband acoustic resonator with a flat-top frequency response. We demonstrate high-resolution spectroscopic measurements of trace amounts of C2H2, NH3 and CO in the entire telecommunications C-band. The method shows a minimum detection limit of 0.6 ppb C2H2 at the measurement time of 100 s, corresponding to the noise equivalent absorption coefficient of 7 × 10-10 cm-1. The proposed cavity-enhanced photoacoustic DCS may open new avenues for ultrasensitive, high-resolution, and multi-species gas detection with widespread applications.

Mid-infrared Ring Interband Cascade Laser: Operation at the Standard Quantum Limit.

Many precision applications in the mid-infrared spectral range have strong constraints based on quantum effects that are expressed in particular noise characteristics. They limit, e.g., sensitivity and resolution of mid-infrared imaging and spectroscopic systems as well as the bit-error rate in optical free-space communication. Interband cascade lasers (ICLs) are a class of mid-infrared lasers exploiting interband transitions in type-II band alignment geometry. They are currently gaining significant importance for mid-infrared applications from < 3 to > 6 µm wavelength, enabled by novel types of high-performance ICLs such as ring-cavity devices. Their noise behavior is an important feature that still needs to be thoroughly analyzed, including its potential reduction with respect to the shot-noise limit. In this work, we provide a comprehensive characterization of λ = 3.8 µm-emitting, continuous-wave ring ICLs operating at room temperature. It is based on an in-depth study of their main physical intensity noise features such as their bias-dependent intensity noise power spectral density and relative intensity noise. We obtained shot-noise-limited statistics for Fourier frequencies above 100 kHz. This is an important result for precision applications, e.g., interferometry or advanced spectroscopy, which benefit from exploiting the advantage of using such a shot-noise-limited source, enhancing the setup sensitivity. Moreover, it is an important feature for novel quantum optics schemes, including testing specific light states below the shot-noise level, such as squeezed states.

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.