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We report a technique based upon the cavity ringdown method that enables to characterize the Brillouin gain coefficient directly in a laser cavity. Material gain, optical cavity parameters and lasing properties can be extracted from measurements whithin a single experiment.

Laser light is confined in a hollow waveguide between two highly reflective mirrors. This waveguide cavity is used to conduct Cavity Ringdown Absorption Spectroscopy of loss mechanisms in the cavity including absorption or scattering by gases, liquid, solids, and/or optical elements.

We have realized a compact optical particle counter utilizing enhancement of light scattering within a high finesse Fabry-Perot optical cavity. In contrast to laser-based approaches such as cavity ringdown spectroscopy we use the light stream from both superluminescent and light-emitting diodes that have no longitudinal coherence. This eliminates the vibration sensitivity that is typical of laser-based cavity methods. The use of the transmission mode of detection allows us to reduce the cavity mirror separation to below 1 cm, with no obvious limit to miniaturization. Typical light scattering instruments are larger, in part due to their sensitivity to background signals from the light source. Our approach paves the way toward a new generation of compact and portable instruments. A simultaneous comparison of the scattering signals with a commercial particle counter shows that our cavity is also sensitive to ultrafine particles below 300 nm diameter that are typically not recorded in such counters., Comment: 13 pages, 6 figures, submitted to Applied Optics

Despite existing for millennia, tuberculosis (TB) remains a persistent global health challenge. A significant obstacle in controlling TB spread is the need for a rapid, portable, sensitive, and accurate diagnostic test. Currently, sputum culture stands as a benchmark test for TB diagnosis. Although highly reliable, it necessitates advanced laboratory facilities and involves considerable testing time. In this context, we present a rapid, portable, and cost-effective optical fiber sensor designed to measure lipoarabinomannan (LAM), a TB biomarker found in patients' urine samples. Our sensing approach is based on the applications of phase shift-cavity ringdown spectroscopy (PS-CRDS) to an optical fiber cavity created by two fiber Bragg gratings. A tapered fiber is spliced inside the optical cavity to serve as the sensing head. We functionalize the tapered fiber surface with anti-LAM antigen CS-35 through a unique chemistry, creating a strong affinity for LAM molecules. We measure the phase difference between the cavity transmission and the reference modulating signal at the cavity output. The measured phase is directly proportional to the injected LAM concentrations in aqueous solutions over the sensing head. Our demonstrated sensor provides a detection limit of 10 pg/mL and a sensitivity of 2.6$^\circ$/ng/mL. This sensor holds promise for numerous applications in the healthcare sector, particularly in low-resource settings., Comment: This paper is submitted to Biomedical Optics Express on 28 Dec 2023

Detection sensitivity is one of the most important attributes to consider during selection of spectroscopic techniques. However, high sensitivity alone is insufficient for spectroscopic measurements in spectrally congested regions. Two-color cavity ringdown spectroscopy (2C-CRDS), based on intra-cavity pump-probe detection, simultaneously achieves high detection sensitivity and selectivity. The technique enables mid-infrared detection of radiocarbon dioxide ($^{14}$CO$_2$) molecules in room-temperature CO$_2$ samples, with better than 10 parts-per-quadrillion (ppq, 10$^{15}$) quantitation accuracy (4 ppq on average). These $highly$-$reproducible$ measurements, which are the most $\it{sensitive}$ and $\it{quantitatively}$ $\it{accurate}$ in the mid-infrared, are accomplished despite the presence of $\it{orders}$-$\it{of}$-$\it{magnitude}$ stronger, one-photon signals from other CO$_2$ isotopologues. This is a major achievement in laser spectroscopy. A room-temperature-operated, compact, and low-cost 2C-CRDS sensor for $^{14}$CO$_2$ benefits a wide range of scientific fields that utilize $^{14}$C for dating and isotope tracing, most notably atmospheric $^{14}$CO$_2$ monitoring to track CO$_2$ emissions from fossil fuels. The 2C-CRDS technique significantly enhances the general utility of high-resolution mid-infrared detection for analytical measurements and fundamental chemical dynamics studies., Comment: 17 pages, 4 figures, 1 table

The Heating Neutral Beam Injectors (HNBs) for ITER will have to deliver 16.7 MW beams of H/D particles at 1 MeV energy. The beams will be produced from H-/D- ions, generated by a radiofrequency plasma source coupled to an ion acceleration system. A prototype of the ITER HNB ion source is being tested in the SPIDER experiment, part of the ITER Neutral Beam Test Facility at Consorzio RFX. Reaching the design targets for beam current density and fraction of coextracted electrons is only possible by evaporating cesium in the source, in particular on the plasma facing grid (PG) of the acceleration system. In this way the work function of the surfaces decreases, significantly increasing the amount of surface reactions that convert neutrals and positive ions into H-/D-. It is then of paramount importance to monitor the density of negative ions and the density of Cs in the proximity of the PG. Monitoring the Cs spatial distribution along the PG is also essential to guarantee the uniformity of the beam current. In SPIDER, this is possible thanks to the Cavity Ringdown Spectroscopy (CRDS) and the Laser absorption Spectroscopy diagnostics (LAS), which provide line-integrated measurements of negative ion density and neutral, ground state Cs density, respectively. The paper discusses the CRDS and LAS measurements as a function of input power and of the magnetic and electric fields used to reduce the coextraction of electrons. Negative ion density data are in qualitative agreement with the analogous measurements in Cs-free conditions. In agreement with simulations, Cs density is peaked in the center of the source; a top/bottom non uniformity is also present. Several effects of plasma on Cs deposition and negative ion production are presented., Comment: 21 pages, 12 figures. Paper (accepted manuscript) following the poster contribution at the SOFT 2022 conference. Published in Fusion Engineering and Design

The measurement science in realizing and disseminating the unit for pressure in the International System of Units (SI), the pascal (Pa), has been the subject of much interest at the National Institute of Standards and Technology (NIST). Modern optical-based techniques for pascal metrology have been investigated, including multi-photon ionization and cavity ringdown spectroscopy. Work is ongoing to recast the pascal in terms of quantum properties and fundamental constants and in so doing, make vacuum metrology consistent with the global trend toward quantum-based metrology. NIST has ongoing projects that interrogate the index of refraction of a gas using an optical cavity for low vacuum, and count background particles in high vacuum to extreme high vacuum using trapped laser-cooled atoms., Comment: 49 pages, 11 figures, review article

The Diffuse Interstellar Bands (DIBs) are a set of ~500 absorption bands that are detected in the spectra of stars with interstellar clouds in the line of sight. DIBs are found from the NUV to the NIR in the spectra of reddened stars spanning different interstellar environments in our local, and in other galaxies. DIB carriers are a significant part of the interstellar chemical inventory. They are stable and ubiquitous in a broad variety of environments and play a unique role in interstellar physics/chemistry. It has long been realized that the solving of the DIB problem requires a strong synergy between astronomical observations, laboratory astrophysics, and astrophysical modeling of line-of-sights. PAHs are among the molecular species that have been proposed as DIB carriers. We will present an assessment of the PAH-DIB model in view of the progress and the advances that have been achieved over the past years through a series of studies involving astronomical observations of DIBs, laboratory simulation of interstellar analogs for neutrals and ionized PAHs, theoretical calculations of PAH spectra and the modelization of diffuse and translucent interstellar clouds. We will present a summary of what has been learned from these complementary studies, the constraints that can now be derived for the PAHs as DIB carriers in the context of the PAH-DIB model and how these constraints can be applied to the EDIBLES project. The spectra of several neutral and ionized PAHs isolated in the gas phase at low temperature have been measured in the laboratory under experimental conditions that mimic interstellar conditions and are compared with an extensive set of astronomical spectra of reddened, early type stars. The comparisons of astronomical and laboratory data provide upper limits for the abundances of specific neutral PAH molecules and ions along specific lines-of-sight. Something that is not attainable from infrared observations alone. We present the characteristics of the laboratory facilities, MIS and COSmIC, that have been developed for this study and discuss the findings resulting from the comparison of the laboratory data with high resolution, high S/N ratio astronomical observations. MIS stands for Matrix Isolation Spectroscopy, a well-proven technique for isolating cold molecular species in inert solid environments. COSmIC stands for Cosmic Simulation Chamber. It combines a supersonic free jet expansion with discharge plasma and high-sensitivity cavity ringdown spectroscopy and time-of-flight mass spectrometry detection tools for the generation and the detection of cold, isolated gas-phase molecules and ions under experimental conditions that closely mimic interstellar conditions. The column densities of the individual neutral PAH molecules and ions probed in these surveys are derived from the comparison of these unique laboratory data with high resolution, high S/N ratio astronomical observations. The comparisons of astronomical and laboratory data lead to clear and unambiguous conclusions regarding the expected abundances for PAHs of various sizes and charge states in the interstellar environments probed in the surveys. Band profile comparisons between laboratory and astronomical spectra lead to information regarding the molecular structures and characteristics associated with the DIB carriers in the corresponding lines-of-sight. These quantitative surveys of neutral and ionized PAHs in the optical range open the way for unambiguous quantitative searches of PAHs and complex organics in a variety of interstellar and circumstellar environments.

The spectra of neutral and ionized PAHs isolated in the gas phase at low temperature have been measured in the laboratory under conditions that mimic interstellar conditions and are compared with a set of astronomical spectra of reddened, early type stars. The comparisons of astronomical and laboratory data provide upper limits for the abundances of neutral PAH molecules and ions along specific lines-of-sight. Something that is not attainable from infrared observations. We present the characteristics of the laboratory facility (COSmIC) that was developed for this study and discuss the findings resulting from the comparison of the laboratory data with high resolution, high S/N ratio astronomical observations. COSmIC combines a supersonic jet expansion with discharge plasma and cavity ringdown spectroscopy and provides experimental conditions that closely mimic the interstellar conditions. The column densities of the individual PAH molecules and ions probed in these surveys are derived from the comparison of the laboratory data with high resolution, high S/N ratio astronomical observations. The comparisons of astronomical and laboratory data lead to clear conclusions regarding the expected abundances for PAHs in the interstellar environments probed in the surveys. Band profile comparisons between laboratory and astronomical spectra lead to information regarding the molecular structures and characteristics associated with the DIB carriers in the corresponding lines-of-sight. These quantitative surveys of neutral and ionized PAHs in the optical range open the way for quantitative searches of PAHs and complex organics in a variety of interstellar and circumstellar environments.

The spectra of several neutral and ionized PAHs isolated in the gas phase at low temperature have been measured in the laboratory under experimental conditions that mimic interstellar conditions and are compared with an extensive set of astronomical spectra of reddened, early type stars [1, 2]. The comparisons of astronomical and laboratory data provide upper limits for the abundances of specific neutral PAH molecules and ions along specific lines-of-sight. Something that is not attainable from infrared observations alone. We present the characteristics of the laboratory facility (COSmIC) that was developed for this study and discuss the findings resulting from the comparison of these unique laboratory data with high resolution, high S/N ratio astronomical observations. COSmIC combines a supersonic free jet expansion with discharge plasma and high-sensitivity cavity ringdown spectroscopy and provides experimental conditions that closely mimic the interstellar conditions. The column densities of the individual neutral PAH molecules and ions probed in these surveys are derived from the comparison of these unique laboratory data with high resolution, high S/N ratio astronomical observations. The comparisons of astronomical and laboratory data lead to clear and unambiguous conclusions regarding the expected abundances for PAHs of various sizes and charge states in the interstellar environments probed in the surveys. Band profile comparisons between laboratory and astronomical spectra lead to information regarding the molecular structures and characteristics associated with the DIB carriers in the corresponding lines-of-sight. These quantitative surveys of neutral and ionized PAHs in the optical range open the way for unambiguous quantitative searches of PAHs and complex organics in a variety of interstellar and circumstellar environments.

Carbonaceous materials play an important role in space. Polycyclic Aromatic Hydrocarbons (PAHs) are a ubiquitous component of the carbonaceous materials. PAHs are the best-known candidates to account for the IR emission bands. They are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge is to reproduce in the laboratory the physical conditions that exist in the emission and absorption interstellar zones. The harsh physical conditions of the ISM -low temperature, collisionless, strong UV radiation fields- are simulated in the laboratory by associating a molecular beam with an ionizing discharge to generate a cold plasma expansion. PAH ions and radicals are formed from the neutral precursors in an isolated environment at low temperature and probed with high-sensitivity cavity ringdown spectroscopy in the NUV-NIR range. Carbon nanoparticles are also formed during the short residence time of the precursors in the plasma and are characterized with time-offlight mass spectrometry. These experiments provide unique information on the spectra of large carbonaceous molecules and ions in the gas phase that can now be directly compared to interstellar and circumstellar observations (IR emission bands, DIBs, extinction curve). These findings also hold great potential for understanding the formation process of interstellar carbonaceous grains. We will review recent progress in the experimental and theoretical studies of PAHs, compare the laboratory data with astronomical observations and discuss the global implications.

Polycyclic Aromatic Hydrocarbons (PAHs) are an important and ubiquitous component of carbon-bearing materials in space. PAHs are the best-known candidates to account for the IR emission bands (UIR bands) and PAH spectral features are now being used as new probes of the ISM. PAHs are also thought to be among the carriers of the diffuse interstellar absorption bands (DIBs). In the model dealing with the interstellar spectral features, PAHs are present as a mixture of radicals, ions and neutral species. PAH ionization states reflect the ionization balance of the medium while PAH size, composition, and structure reflect the energetic and chemical history of the medium. A major challenge for laboratory astrochemistry is to reproduce (in a realistic way) the physical conditions that are associated with the emission and absorption interstellar zones. An extensive laboratory program has been developed at NASA Ames to assess the physical and chemical properties of PAHs in such environments and to describe how they influence the radiation and energy balance in space and the interstellar chemistry. PAHs, neutrals and ions, are expanded through a pulsed discharge nozzle (PDN) and probed with high-sensitivity cavity ringdown spectroscopy (CRDS). These laboratory experiments provide unique information on the spectra of free, cold large carbon molecules and ions in the gas phase from the ultraviolet and visible range to the near-infrared range. Intrinsic band profiles and band positions of cold gas-phase PAHs can now be measured with high-sensitivity spectroscopy and directly compared to the astronomical data. Preliminary conclusions from the comparison of the laboratory data with astronomical observations of interstellar and circumstellar environments will also be discussed.

The term plasma process diagnostics (PPD) refers to a spectroscopic technique and sensing hardware that have been proposed for monitoring plasma processes used to fabricate electronic devices that feature sizes as small as several nanometers. Nanometer dimensions are characteristic of the quantum level of miniaturization, where single impurity atoms or molecules can drastically change the local properties of the nanostructures. Such changes may be purposely used in nanoscale design but may also be extremely damaging or cause improper operation of the fabricated devices. Determination of temperature and densities of reactants near the developing features is important, since the structural synthesis is affected by characteristics of the local microenvironment. Consequently, sensors capable of nonintrusive monitoring with high sensitivity and high resolution are essential for real-time atomistic control of reaction kinetics and minimizing trace contamination in plasma processes used to fabricate electronic nanodevices. Such process-monitoring sensors are required to be compact, multiparametric, and immune to the harsh environments of processing plasmas. PPD is intended to satisfy these requirements. The specific technique used to implement plasma diagnostics with a PPD sensor would be an advanced version of continuous-wave cavity-ringdown spectroscopy (CW-CRDS) capable of profiling spectral line broadenings in order to derive both Doppler and Stark components. CRDS is based on measurements of the rate of absorption of laser light in an optical resonator. The ultimate sensitivity results from a very long absorption path length within the cavity and immunity to variations in incident laser intensity. The proposed version of this technique would involve the use of multiplexing tunable laser diodes and an actively modulated high-reflectivity optical resonator, thus offering a synergistic combination of simplicity, compactness, high sensitivity, and high resolution. The multiplexing capabilities of diode lasers could be utilized to make the PPD sensor a single, simple, compact, and inexpensive tool for the acquisition of multiparametric data. A PPD sensor would be capable of continuous measurement of such physical parameters as gas temperature, gas velocity, electron number density, and absolute densities of reacting chemical species. A laser beam can be easily adjusted to analyze the immediate vicinity of the growing nanostructures (or features etched down) in real time. The absorption enhancement in an optical cavity would afford the sensitivity needed for measurement of the temperature and densities of species at concentrations significantly lower than measurable by other nonintrusive techniques. It is anticipated that fully developed PPD sensors would enable simultaneous measurement of local temperature and determination of plasma species responsible for the synthesis and functionalization of nanodevices. These sensors would also enable tracking the pathways and origins of damaging contaminants, thereby providing feedback for adjustment of processes to optimize them and reduce contamination. The PPD sensors should also be useful for optimization of conventional microelectronics manufacturing plasma processes. Going beyond plasma processes for fabrication of electronic devices, PPD sensors could be used for monitoring of atoms, molecules, ions, radicals, clusters, and particles in a variety of other settings, including outer space. Because of their high sensitivity, such sensors could also prove useful for detecting traces of illegal drugs and explosives.

In a collaboration with the Mats Larsson group from Stockholm, we carried out a new measurement of the rate of dissociative recombination of H(sup *, sub j), using a new pulsed supersonic beam source of rotationally cold H(sup *, sub j). This source was first designed and characterized in our lab by IR cavity ringdown spectroscopy, determining a rotationaYtranslationa1 temperature of 20-60K, depending on conditions. This new source was then taken to Stockholm for the recombination rate studies at the CRYRING storage ring. The recombination rate constant measured against temperature yields values consistent with the most recent calculations, whereas previous experimental measurements varied over a range of 10(exp 4) and were poor agreement with theory. This is a crucial achievement for understanding the ion chemistry of diffuse clouds. Moreover, this result in combination with recent observations implies a greatly enhanced (factor of 40) cosmic ray ionization rate in a diffuse cloud (zeta Persei) relative to previous studies. The implications of this are discussed in our recent Nature paper. An enhanced cosmic-ray flux towards zeta Persei inferred from a laboratory study of the H(sup *, sub j)-e(sup -) recombination rate.

The gas-phase electronic absorption spectra of the naphthalene (C10H8(+)) and acenaphthene (C12H10(+)) cations have been measured in the visible range in a free 10 jet planar expansion in an attempt to collect data in an astrophysically relevant environment. The direct absorption spectra of two out of four bands measured of the gas-phase cold naphthalene cation along with the gas-phase vibronic absorption spectrum of the cold acenaphthene cation are reported for the first time. The study has been carried out using the ultrasensitive and versatile technique of cavity ringdown spectroscopy (CRDS) coupled to a pulsed discharge slit nozzle (PDN). The new CRDS-PDN set up is described and its characteristics are evaluated. The direct-absorption spectra of the PAH ions are discussed and compared to the gas-phase and solid-phase data available in the literature. The analysis of the results show that cold, free flying PAH ions are generated in the argon discharge primarily through soft Penning ionization. This enables the intrinsic band profiles to be measured, a key requirement for astrophysical applications.

The progress in the development of a sensor for the detection of trace air constituents to monitor spacecraft air quality is reported. A continuous-wave (cw), external-cavity tunable diode laser centered at 1.55 micrometers is used to pump an optical cavity absorption cell in cw-cavity ringdown spectroscopy (cw-CRDS). Preliminary results are presented that demonstrate the sensitivity, selectivity and reproducibility of this method. Detection limits of 2.0 ppm for CO, 2.5 ppm for CO2, 1.8 ppm for H2O, 19.4 ppb for NH3, 7.9 ppb for HCN and 4.0 ppb for C2H2 are calculated.

Aerosols are important contributors to the radiative forcing in the atmosphere. Much of the uncertainty in our knowledge of climate forcing is due to uncertainties in the radiative forcing due to aerosols as illustrated in the IPCC reports of the last ten years. Improved measurement of aerosol optical properties, therefore, is critical to an improved understanding of atmospheric radiative forcing. Additionally, attempts to reconcile in situ and remote measurements of aerosol radiative properties have generally not been successful. This is due in part to the fact that it has been impossible to measure aerosol extinction in situ in the past. In this presentation we introduce a new instrument that employs the techniques used in cavity ringdown spectroscopy to measure the aerosol extinction and scattering coefficients in situ. A prototype instrument has been designed and tested in the lab and the field. It is capable of measuring aerosol extinction coefficient to 2x10(exp -6) per meter. This prototype instrument is described and results are presented.