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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 (14C) is playing a crucial role in this scenario because it is one of the so-called difficult to measure isotopes; currently, 14C 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 14C 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) F14C and 30.951(7) F14C 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) F14C (∼0.7 ppt) from a concrete sample originating from an external wall of the Ispra-1 nuclear research reactor currently in the decommissioning phase. [ABSTRACT FROM AUTHOR]

Optical frequency combs generated by quantum cascade lasers have recently been demonstrated in the mid and far infrared, but a detailed analysis of the possibility of a fine control of the emission to use them for high-resolution spectroscopy and metrology applications is still missing. In this manuscript the attempt of frequency stabilizing a mid-infrared quantum cascade laser comb (QCL-comb) against a metrological mid-infrared intracavity-difference-frequency-generated comb through a single phase-locking chain acting on the driving current is presented. Following a brief derivation, simple relations between the QCL-comb frequency parameters and optical quantities such as the refractive index have been found and used to observe how the locking affects the physics of the system. The conclusion is that the current locking essentially acts on the effective refractive index to reduce the offset fluctuations (common noise), but does not sensitively affect the group refractive index and the mode spacing. Nonetheless, the overall single QCL-comb tooth linewidth is reduced from 500 kHz down to values ranging from 1 to 23 kHz on a 40 ms time scale. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

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. [ABSTRACT FROM AUTHOR]

The infrared spectrum of the (0111–0110) ro-vibrational band of12C16O2in the range 2306–2312 cm−1is investigated with saturated-absorption sub-Doppler spectroscopy. The absolute frequencies of six transitions belonging to the P-branch of this band are measured by recording their Lamb-dip features in a pump-probe detection scheme employing a room-temperature quantum cascade laser. The laser is phase-locked to a subkilohertz-linewidth difference-frequency-generated radiation source, which is referenced to an optical frequency comb synthesiser. The achieved relative uncertainties range from 1×10−11to 5×10−11, improving by three to four orders of magnitude the previous tabulated values for such frequencies. Moreover, thanks to this precision level, self-pressure-shift coefficients due to collisional processes of CO2molecules are reported for the first time. [ABSTRACT FROM AUTHOR]

The infrared spectrum of the rare isotopologue has been investigated in the range 2190–2250 cm−1 with a frequency-comb-referenced cavity ring-down spectrometer. Thirty-three ro-vibrational transitions of the ν3 fundamental band have been detected. Their absolute frequency was measured with a relative uncertainty ranging from to . The experimental frequencies were fitted to the conventional Hamiltonian of a linear molecule and a new set of spectroscopic parameters for the fundamental vibrational state has been improved for this species. [ABSTRACT FROM PUBLISHER]

Quantum cascade lasers (QCLs) are becoming a key tool in several advanced experiments in the field of precision molecular spectroscopy and absolute frequency metrology. In view of this, a thorough control of their emission properties must be achieved, including a narrow linewidth as well as a high frequency-stability combined with referencing to a primary standard. Here, we give a review on recent developments and next perspectives in this scope, with particular regard to the use of QCLs in fundamental physics spectroscopic searches. [ABSTRACT FROM AUTHOR]