In-situ analysis of combustion aerosol using a supercontinuum lidar.

We report real-time monitoring of coarse aerosol particle distribution in a 9 m wide full-scale industrial boiler using a broadband supercontinuum lidar. The technique utilizes the light backscattered from the aerosol to map the extinction profile using the Klett inversion method, with measured extinction values of 0.04 - 0.2 m-1 across the furnace. The technique further exploits differential absorption of water molecules in the 1.25 - 1.5 µm region to map the water vapor concentration profile in the furnace up to a distance of 3.9 m with a spatial resolution of 30 cm. We also take advantage of the strong reflection from the boiler back-wall to simultaneously measure the average water vapor temperature and concentration in the boiler in good agreement with reference readings from the boiler. Our results open novel perspectives for versatile 3D profiling of flue gas parameters and other industrial process analysis.

Mid-infrared hyperspectral sensor based on MEMS Fabry-Pérot interferometer for stand-off sensing applications.

We report a novel hyperspectral sensor employing a Fabry-Pérot interferometer based on micro-electro-mechnical system and a custom mid-infrared supercontinuum laser. The Fabry-Pérot interferometer allows on-axis filtering, of spectral components of supercontinuum light backscattered from a target, with a spectral resolution of about 25 nm. We demonstrated hyperspectral identification of black polypropylene (PP) and polyethylene (PE500) using the 3-3.5 [Formula: see text]m region of the supercontinuum spectrum and a corresponding measurement rate of 62.5 spectra / s. The resulted spectra show excellent agreement with the reference based on an FTIR spectrometer. Furthermore, we showed that the coloring of the plastics has no effect on their identification at this wavelength range.

Sensitive multi-species photoacoustic gas detection based on mid-infrared supercontinuum source and miniature multipass cell.

We report multipass broadband photoacoustic spectroscopy of trace gases in the mid-infrared. The measurement principle of the sensor relies on supercontinuum-based Fourier transform photoacoustic spectroscopy (FT-PAS), in which a scanning interferometer modulates the intensity of a mid-infrared supercontinuum light source and a cantilever microphone is employed for sensitive photoacoustic detection. With a custom-built external Herriott cell, the supercontinuum beam propagates ten times through a miniature and acoustically non-resonant gas cell. The performance of the FT-PAS system is demonstrated by measuring the fundamental C-H stretch bands of various hydrocarbons. A noise equivalent detection limit of 11 ppb is obtained for methane (40 s averaging time, 15 µW cm-1 incident power spectral density, 4 cm-1 resolution), which is an improvement by a factor of 12 compared to the best previous FT-PAS systems. High linearity and good stability of the sensor provide reliable identification of individual species from a gas mixture with strong spectral overlap, laying the foundation for sensitive and selective multi-species detection in small sample volumes.

Elemental analysis of single ambient aerosol particles using laser-induced breakdown spectroscopy.

Analysing the composition of aerosol particles is essential when studying their health effects, sources and atmospheric impacts. In many environments the relevant particles occur in very low concentrations, meaning that their analysis requires efficient single particle techniques. Here we introduce a novel method to analyse the elemental composition of single aerosol particles sampled directly from the aerosol phase using size amplification aided aerosol charging (SAAC), linear electrodynamic quadrupole (LEQ) and laser-induced breakdown spectroscopy. We present results of the charging and focusing efficiencies of the SAAC and of the LEQ, and a proof-of-concept of the analysis method. The proof-of-concept test series was conducted with particle diameters down to 300 nm, sampled directly from the aerosol phase. The method shows unprecedented performance for spectroscopic submicron particle analysis from arbitrarily low concentrations and has exceptional potential for a portable analysis platform for various applications in the field of aerosol research.

Supercontinuum intensity noise coupling in Fourier transform photoacoustic spectroscopy.

We investigate the noise transfer mechanism from the light source intensity fluctuations to the acoustic signal in Fourier transform photoacoustic spectroscopy (FT-PAS). This noise coupling is expected to be reduced in FT-PAS compared with conventional Fourier transform spectroscopy, as only the specific spectral components that are absorbed by the probed sample contribute to the noise level. We employ an incoherent supercontinuum (SC) light source in our experiments and observe a linear relation between the sample gas concentration and the detected noise level, which significantly reduces the influence of the SC noise on the detection limit. Based on our experimental results, we derive a model for the noise level, which establishes the foundation for practical sensitive implementation of FT-PAS.

Maskless fabrication of plasmonic metasurfaces in polymer film using a spatial light modulator.

We demonstrate a high-speed optical technique to fabricate plasmonic metasurfaces in a polymer film. The technique is based on a programmable spatial light modulator, which is used to spatially control the photoreduction sites of gold ions in a polyvinyl alcohol film doped with a gold precursor. After irradiation, annealing was used to induce the growth of nanoparticles, producing plasmonic microstructures. Using a 473 nm excitation wavelength, microscopic plasmonic gratings, and meta-atom arrays with arbitrary orientations, an effective nanostructure size of ∼700nm and constituent nanoparticles with average size of ∼37nm were created. The technique enables a cost-effective and straightforward light-based approach to fabricate plasmonic metasurfaces with tunable properties.

Broadband Laser-Based Infrared Detector for Gas Chromatography.

Cantilever-enhanced photoacoustic spectroscopy coupled with gas chromatography is used to quantitatively analyze a mixture of alcohols in a quasi-online manner. A full identification and quantification of all analytes are achieved based on their spectral fingerprints using a widely tunable continuous-wave laser as a light source. This can be done even in the case of interfering column/septum bleed or simultaneously eluted peaks. The combination of photoacoustic spectroscopy and gas chromatography offers a viable solution for compact and portable instruments in applications that require straightforward analyses with no consumables.

Sequential Collinear Photofragmentation and Atomic Absorption Spectroscopy for Online Laser Monitoring of Triatomic Metal Species.

Industrial chemical processes are struggling with adverse effects, such as corrosion and deposition, caused by gaseous alkali and heavy metal species. Mitigation of these problems requires novel monitoring concepts that provide information on gas-phase chemistry. However, selective optical online monitoring of the most problematic diatomic and triatomic species is challenging due to overlapping spectral features. In this work, a selective, all-optical, in situ gas-phase monitoring technique for triatomic molecules containing metallic atoms was developed and demonstrated with detection of PbCl2. Sequential collinear photofragmentation and atomic absorption spectroscopy (CPFAAS) enables determination of the triatomic PbCl2 concentration through detection of released Pb atoms after two consecutive photofragmentation processes. Absorption cross-sections of PbCl2, PbCl, and Pb were determined experimentally in a laboratory-scale reactor to enable calibration-free quantitative determination of the precursor molecule concentration in an arbitrary environment. Limit of detection for PbCl2 in the laboratory reactor was determined to be 0.25 ppm. Furthermore, the method was introduced for in situ monitoring of PbCl2 concentration in a 120 MWth power plant using demolition wood as its main fuel. In addition to industrial applications, the method can provide information on chemical reaction kinetics of the intermediate species that can be utilized in reaction simulations.

Single-frequency 100†ns / 0.5 mJ laser pulses from all-fiber double clad ytterbium doped tapered fiber amplifier.

High peak power, narrow linewidth sources continue to be in high demand. Fiber amplifiers are a compelling option to scale peak power of long 100-ns-pulses because of their compact size and robustness. Unfortunately, stimulated Brillouin scattering (SBS) limits peak power of narrow linewidth fiber sources causing instability. We demonstrate SBS suppression for 130-ns pulses from a 5 MHz linewidth seed laser in a fiber amplifier by using tapered fiber with large 50 µm diameter core in the output. The longitudinal change in the core diameter induces frequency shift in the SBS gain peak and the back-travelling Stokes wave is suppressed towards smaller core. We reach 2.2 kW peak power with 18.7 dB polarization extinction ratio and record breaking 4 kW peak power by exciting both polarization states of the polarization maintaining tapered fiber. The output beam quality equals to single mode fibers with M2 = 1.08.

Dynamic Enhancement of Nitric Oxide Radioluminescence with Nitrogen Purge.

Remote detection of alpha radiation is commonly realised by collecting the light, the radioluminescence, that is produced when alpha particles are stopped in air. Radioluminescence of nitric oxide (NO) is primarily emitted between 200 nm and 300 nm, which makes it possible to use it for remote detection under daylight conditions. Quenching by ambient oxygen and water vapour, however, makes it generally difficult to effectively create NO radioluminescence. We present the detection of intense NO radioluminescence in ambient air under standard indoor lighting conditions using a nitrogen purge. The nitrogen contained NO impurities that were intrinsic to the gas and had not explicitly been added. We study the mechanisms that govern the NO radioluminescence production and introduce a model to describe the dynamics of the process. The level of NO contained in the gas was found to determine how successful a purge can be. We conclude by discussing possible applications of the technique in nitrogen-flushed gloveboxes at nuclear facilities where NO concentration of 100 ppb-1 ppm would be sufficient for efficient optical alpha radiation detection in standard lighting conditions.

Short-range supercontinuum-based lidar for temperature profiling.

We developed a short-range light detection and ranging system using a supercontinuum (SC) source spectrally tailored to cover the ro-vibrational transition energies of desired components of a flue gas. The system enables remote measurements of the gas parameters, including temperature and concentration which play a key role in the performance of combustion power plants. The technique requires only one inspection window and, thus, can be used in combustion units with limited access. It exploits differential absorption between specific wavelength bands of the gas absorption spectrum. The transmittance of an individual wavelength band is derived from the detected backscattered temporal intensity of the SC pulses. We demonstrate water vapor temperature measurement in the range of 400°C-900°C in a laboratory furnace with the use of only two wavelength bands. Using more than two wavelength bands, the technique can be further extended to simultaneously measure temperature and concentration. By varying the direction of the incident beam in a non-parallel plane, a full 3D profile is also obtainable.

Alpha Radiation-Induced Luminescence by Am-241 in Aqueous Nitric Acid Solution.

When exposed to air, alpha particles cause the production of light by exciting the molecules surrounding them. This light, the radioluminescence, is indicative of the presence of alpha radiation, thus allowing for the optical sensing of alpha radiation from distances larger than the few centimeters an alpha particle can travel in air. While the mechanics of radioluminescence in air and other gas compositions is relatively well understood, the same cannot be said about the radioluminescence properties of liquids. Better understanding of the radioluminescence properties of liquids is essential to design methods for the detection of radioactively contaminated liquids by optical means. In this article, we provide radioluminescence images of Am-241 dissolved in aqueous nitric acid ( HNO 3 ) solution and present the recorded radioluminescence spectrum with a maximum between 350 nm and 400 nm , and a steep decrease at the short wavelength side of the maximum. The shape of the spectrum resembles a luminescence process rather than Cerenkov light, bremsstrahlung, or other mechanisms with broadband emission. We show that the amount of light produced is about 150 times smaller compared to that of the same amount of Am-241 in air. The light production in the liquid is evenly distributed throughout the sample volume with a slight increase on the surface of the liquid. The radioluminescence intensity is shown to scale linearly with the Am-241 concentration and not be affected by the HNO 3 concentration.

Optical frequency comb photoacoustic spectroscopy.

We report the first photoacoustic detection scheme using an optical frequency comb-optical frequency comb photoacoustic spectroscopy (OFC-PAS). OFC-PAS combines the broad spectral coverage and the high resolution of OFCs with the small sample volume of cantilever-enhanced PA detection. In OFC-PAS, a Fourier transform spectrometer (FTS) is used to modulate the intensity of the exciting comb source at a frequency determined by its scanning speed. One of the FTS outputs is directed to the PA cell and the other is measured simultaneously with a photodiode and used to normalize the PA signal. The cantilever-enhanced PA detector operates in a non-resonant mode, enabling detection of a broadband frequency response. The broadband and the high-resolution capabilities of OFC-PAS are demonstrated by measuring the rovibrational spectra of the fundamental C-H stretch band of CH4, with no instrumental line shape distortions, at total pressures of 1000 mbar, 650 mbar, and 400 mbar. In this first demonstration, a spectral resolution two orders of magnitude better than previously reported with broadband PAS is obtained, limited by the pressure broadening. A limit of detection of 0.8 ppm of methane in N2 is accomplished in a single interferogram measurement (200 s measurement time, 1000 MHz spectral resolution, 1000 mbar total pressure) for an exciting power spectral density of 42 µW/cm-1. A normalized noise equivalent absorption of 8 × 10-10 W cm-1 Hz-1/2 is obtained, which is only a factor of three higher than the best reported with PAS based on continuous wave lasers. A wide dynamic range of up to four orders of magnitude and a very good linearity (limited by the Beer-Lambert law) over two orders of magnitude are realized. OFC-PAS extends the capability of optical sensors for multispecies trace gas analysis in small sample volumes with high resolution and selectivity.

Machine learning analysis of extreme events in optical fibre modulation instability.

A central research area in nonlinear science is the study of instabilities that drive extreme events. Unfortunately, techniques for measuring such phenomena often provide only partial characterisation. For example, real-time studies of instabilities in nonlinear optics frequently use only spectral data, limiting knowledge of associated temporal properties. Here, we show how machine learning can overcome this restriction to study time-domain properties of optical fibre modulation instability based only on spectral intensity measurements. Specifically, a supervised neural network is trained to correlate the spectral and temporal properties of modulation instability using simulations, and then applied to analyse high dynamic range experimental spectra to yield the probability distribution for the highest temporal peaks in the instability field. We also use unsupervised learning to classify noisy modulation instability spectra into subsets associated with distinct temporal dynamic structures. These results open novel perspectives in all systems exhibiting instability where direct time-domain observations are difficult.

Broadband cantilever-enhanced photoacoustic spectroscopy in the mid-IR using a supercontinuum.

We demonstrate cantilever-enhanced photoacoustic spectroscopy in the mid-infrared using a supercontinuum source. The approach is broadband and allows for higher photoacoustic signal intensity and an enhanced signal-to-noise ratio as compared to systems employing conventional black body radiation sources. Using this technique, we perform spectroscopic measurements of the full ro-vibrational band structure of water vapor at 1900 nm and methane at 3300 nm with relative signal enhancement factors of 70 and 19, respectively, when compared to measurements that use the black body radiation source. Our results offer a novel perspective for photoacoustic detection opening the door to sensitive broadband analyzers in the mid-infrared spectral region.

Intense radioluminescence of NO/N2-mixture in solar blind spectral region.

Luminescence in air induced by alpha particle emitters can be used to optically detect radioactive contamination from distances that surpass the range of the alpha radiation itself. Alpha particles excite nitrogen molecules in air and the relaxation creates a faint light emission. When the composition of the gases surrounding the alpha particle emitter is altered then the luminescence spectrum changes. In this work, we report the creation of an intense light emission in the wavelength regime below 300 nm originating from alpha particle excited nitric oxide (NO). The light yield has been investigated as a function of the NO concentration in an N2 atmosphere. Unlike the emission from molecular nitrogen, NO emits at wavelengths shorter than 300 nm, where solar background and artificial lighting are negligible, thus enabling optical detection of alpha radiation even under bright lighting conditions. We show that the radioactively induced NO emission reaches its maximum intensity at a concentration of 50 ppm of NO diluted in N2. At this concentration, the strongest emission line of NO is about 25 times more intense than the most intense line of N2 radioluminescence. Lastly, we discuss potential applications and limitations of the technique.

Enhanced self-mixing interferometry based on volume Bragg gratings and laser diodes emitting at 405-nm wavelengths.

Self-mixing interferometry (SMI) represents a robust, self-aligned technique for metrology applications. Recently, it has been shown that the detection of the frequency-modulated (FM) signal enhances the conventional SMI signal based on the amplitude modulation. Here, an all-optical, simple and effective alternative approach to detect the FM self-mixing signal is presented. We demonstrate the enhanced self-mixing approach using a laser diode emitting at 405 nm and a volume Bragg grating (VBG) to map frequency to intensity modulations for further optical detection. Our approach overcomes the spectral range limitation of the edge filtering approach based on molecular absorption filters, since the VBGs can be fabricated at any spectral range.

Micropatterning of silver nanoclusters embedded in polyvinyl alcohol films.

Direct laser writing has been utilized to fabricate highly photostable fluorescent nanocluster microstructures in an organic polymer poly(methacrylic acid), where the carboxyl functional group is reported to play a vital role in nanocluster stabilization. In this Letter, we demonstrate that not only the polymer containing the carboxyl functional group, but also the polymer comprising the hydroxyl group, namely polyvinyl alcohol (PVA), can act as an appropriate stabilizer matrix for laser-induced synthesis and patterning of silver nanoclusters. The as-formed nanoclusters in the PVA film exhibit broadband emission and photostability comparable to the nanoclusters formed in the poly(methacrylic acid) polymer. As PVA is a widely used, nontoxic, biocompatible and biodegradable polymer, the technique of patterning fluorescent nanoclusters in PVA thin films is expected to find numerous applications in fields like fluorescence imaging, biolabeling, and sensing.

Detection of single microparticles in airflows by edge-filter enhanced self-mixing interferometry.

A laser Doppler velocimetry (LDV) sensor using the edge-filter enhanced self-mixing interferometry (ESMI) is presented based on speed measurements of single microparticles. The ESMI detection utilizes an acetylene edge-filter that maps the frequency modulation of a semiconductor laser into an intensity modulation as the laser wavelength is tuned to the steep edge of the absorption profile. In this work, the ESMI signal was analyzed for aerosol particles of different sizes from 1 µm to 10 µm at a distance of 2.5 m. At this operation range, the signal from single particles of all sizes was successfully acquired enabling particle velocity measurements through the Doppler shifted frequency along the beam axis. For the particular case of 10 µm particles, single aerosol particles were still detected at an unprecedented range of 10 m. A theoretical treatment describing the relation between Mie scattering theory and the self-mixing phenomenon on single-particle detection is presented supporting the experimental results. The results show that the edge-filter enhanced self-mixing technique opens new possibilities for self-mixing detection where longer ranges, lower backscattering laser powers and higher velocities are involved. For example, it can be used as a robust and inexpensive anemometer for LDV applications for airflows with low-number density of microparticles.