Laser Spectroscopy Research Articles

Precise Exhaust Gas Measurement Based on Laser Spectroscopy

Precise Exhaust Gas Measurement Based on Laser Spectroscopy

Laser spectroscopy and crystal field analysis of energy level structure of Tm3+ ions in SrY2O4 crystal

Site-selective laser spectroscopy study of the multi-site SrY2O4:Tm3+ crystal (0.05 at.%) show that two types of impurity centers of Tm3+ ions are predominantly formed. The Stark sublevel patterns of the 3H6, 3H5, 3F4, 3H4, 3F3, and 1G4 multiplets have been determined. Calculations of the energy level structure for Tm3+ ions at Y1 and Y2 lattice sites have been carried out in the framework of the crystal-field theory. The obtained calculation results agree with the measured energy spectra, supporting an assignment of spectra to Tm3+ ions at Y1 and Y2 lattice sites. To verify the correctness of the performed calculations, the field dependencies of the magnetization along the crystallographic a, b and c axes and the temperature dependence of the magnetization in the magnetic field applied along the c-axis of the SrY2O4:Tm3+ (0.5 at.%) crystal were measured. The set of crystal-field parameters obtained in this work made it possible to fully describe the measured magnetization dependences.

A wideband, high-resolution vector spectrum analyzer for integrated photonics

The analysis of optical spectra—emission or absorption—has been arguably the most powerful approach for discovering and understanding matter. The invention and development of many kinds of spectrometers have equipped us with versatile yet ultra-sensitive diagnostic tools for trace gas detection, isotope analysis, and resolving hyperfine structures of atoms and molecules. With proliferating data and information, urgent and demanding requirements have been placed today on spectrum analysis with ever-increasing spectral bandwidth and frequency resolution. These requirements are especially stringent for broadband laser sources that carry massive information and for dispersive devices used in information processing systems. In addition, spectrum analyzers are expected to probe the device’s phase response where extra information is encoded. Here we demonstrate a novel vector spectrum analyzer (VSA) that is capable of characterizing passive devices and active laser sources in one setup. Such a dual-mode VSA can measure loss, phase response, and dispersion properties of passive devices. It also can coherently map a broadband laser spectrum into the RF domain. The VSA features a bandwidth of 55.1 THz (1260–1640 nm), a frequency resolution of 471 kHz, and a dynamic range of 56 dB. Meanwhile, our fiber-based VSA is compact and robust. It requires neither high-speed modulators and photodetectors nor any active feedback control. Finally, we employ our VSA for applications including characterization of integrated dispersive waveguides, mapping frequency comb spectra, and coherent light detection and ranging (LiDAR). Our VSA presents an innovative approach for device analysis and laser spectroscopy, and can play a critical role in future photonic systems and applications for sensing, communication, imaging, and quantum information processing.

Chemical sensing of common microorganisms found in biopharmaceutical industries using MIR laser spectroscopy and multivariate analysis.

Mid-infrared laser spectroscopy was used to investigate common bacteria encountered in biopharmaceutical industries. The study involved the detection of bacteria using quantum cascade laser spectroscopy coupled to a grazing angle probe (QCL-GAP). Substrates similar to surfaces commonly used in biopharmaceutical industries were used as support media for the samples. Reflectance measurements were assisted by Multivariate Analysis (MVA) to assemble a powerful spectroscopic technique with classification and identification resources. The species analyzed, Staphylococcus aureus, Staphylococcus epidermidis, and Micrococcus luteus, were used to challenge the technique's capability to discriminate from microorganisms of the same family. Principal Components Analysis and Partial Least Squares-Discriminant Analysis differentiated between the bacterial species, using QCL-GAP-MVA as the reference. Spectral differences in the bacterial membrane were used to determine if these microorganisms were present in the samples analyzed. Results herein provided effective discrimination for the bacteria under study with high sensitivity and specificity.

Generation of 2.8 µm fiber laser using an Erbium‐doped ZBLAN double‐clad fiber in a linear‐cavity‐free space experimental setup

AbstractMid‐infrared (MIR) fiber lasers are highly demand after for a variety of technological applications, including uses such as laser surgery, frequency metrology, and spectroscopy. This paper demonstrates a stable continuous‐wave laser operation in the 2.8 µm using an Er3+‐doped ZBLAN fiber operating in a free space experimental setting. A laser output power of 12.4 mW was attained in a linear cavity when this fiber was pumped at 2.9 W of 980 nm laser diode.

Fractionation of Methane Isotopologues during Preparation for Analysis from Ambient Air.

Preconcentration of methane (CH4) from air is a critical sampling step in the measurement of singly and doubly substituted isotopologue ratios. We demonstrate the potential for isotope fractionation during preconcentration onto and elution from the common trapping material HayeSep-D and investigate its significance in laser spectroscopy measurements. By altering the trapping temperature for adsorption, the flow direction of CH4 through the trap and the time at which CH4 is eluted during a desorption temperature ramp, we explain the mechanisms behind fractionation affecting δ13C(CH4) and δ2H(CH4). The results highlight that carbon isotope fractionation is driven by advection and diffusion, while hydrogen isotope fractionation is driven by the interaction of CH4 with the adsorbing material (tending to smaller isotopic effects at higher temperatures). We have compared the difference between the measured isotope ratio of sample gases (compressed whole air and a synthetic mixture of CH4 at ambient amount fraction in an N2 matrix) and their known isotopic composition. An open-system Rayleigh model is used to quantify the magnitude of isotopic fractionation affecting measured δ13C(CH4) and δ2H(CH4), which can be used to calculate the possible magnitude of isotopic fractionation given the recovery percentage. These results provide a quantitative understanding of isotopic fractionation during the sample preparation of CH4 from ambient air. The results also provide valuable insights applicable to other cryogenic preconcentration systems, such as those for measurements that probe the distribution of rarer isotopologues.

Mid-infrared trace detection with parts-per-quadrillion quantitation accuracy: Expanding frontiers of radiocarbon sensing

Detection sensitivity is a critical characteristic 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. This combination enables mid-infrared detection of radiocarbon dioxide ([Formula: see text]CO[Formula: see text]) molecules in room-temperature CO[Formula: see text] samples, with 1.4 parts-per-quadrillion (ppq, 10[Formula: see text]) sensitivity (average measurement precision) and 4.6-ppq quantitation accuracy (average calibrated measurement error for 21 samples from four separate trials) demonstrated on samples with [Formula: see text]C/C up to [Formula: see text]1.5[Formula: see text] natural abundance ([Formula: see text]1,800 ppq). These highly reproducible measurements, which are the most sensitive and quantitatively accurate in the mid-infrared, are accomplished despite the presence of orders-of-magnitude stronger, one-photon signals from other CO[Formula: see text] isotopologues. This is a major achievement in laser spectroscopy. A room-temperature-operated, compact, and low-cost 2C-CRDS sensor for [Formula: see text]CO[Formula: see text] benefits a wide range of scientific fields that utilize [Formula: see text]C for dating and isotope tracing, most notably atmospheric [Formula: see text]CO[Formula: see text] monitoring to track CO[Formula: see text] 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.

Tunable non-polarizing optical bandpass filtering in prism pair coupled planar optical waveguide.

A tunable non-polarizing optical bandpass filter structure, comprising a prism pair coupled planar optical waveguide (POW), is demonstrated, by changing the incident angle of the filter. Experimental measurements show that pass bands for both TM and TE polarized waves are present in the filter simultaneously, and the two passbands overlap on each other. The overlapping of the two passbands can be sustainable for the peak wavelength from 623 to 852 nm as the incident angle of the light tuned within 2°. This POW based optical bandpass filter can be potentially applicable in various fields of optical and laser spectroscopies.

Frequency-comb-linearized, widely tunable lasers for coherent ranging

Tunable lasers, with the ability to continuously vary their emission wavelengths, have found widespread applications across various fields such as biomedical imaging, coherent ranging, optical communications, and spectroscopy. In these applications, a wide chirp range is advantageous for large spectral coverage and high frequency resolution. Besides, the frequency accuracy and precision also depend critically on the chirp linearity of the laser. While extensive efforts have been made on the development of many kinds of frequency-agile, widely tunable, narrow-linewidth lasers, wideband yet precise methods to characterize and linearize laser chirp dynamics are also demanded. Here we present an approach to characterize laser chirp dynamics using an optical frequency comb. The instantaneous laser frequency is tracked over terahertz bandwidth at 1 MHz intervals. Using this approach we calibrate the chirp performance of 12 tunable lasers from Toptica, Santec, New Focus, EXFO, and NKT that are commonly used in fiber optics and integrated photonics. In addition, with acquired knowledge of laser chirp dynamics, we demonstrate a simple frequency-linearization scheme that enables coherent ranging without any optical or electronic linearization unit. Our approach not only presents novel wideband, high-resolution laser spectroscopy, but is also critical for sensing applications with ever-increasing requirements on performance.

Highly sensitive mid-infrared methane remote sensor using a deep neural network filter.

A novel mid-infrared methane remote sensor integrated on a movable platform based on a 3.291-µm interband cascade laser (ICL) and wavelength modulation spectroscopy (WMS) is proposed. A transmitting-receiving coaxial, visualized optical layout is employed to minimize laser energy loss. Using a hollow retro-reflector remotely deployed as a cooperative target, the atmospheric average methane concentration over a 100-meter optical range is measured with high sensitivity. A deep neural network (DNN) filter is used for second harmonic (2f) signal denoising to compensate for the performance shortcomings of conventional filtering. Allan deviation analysis indicated that after applying the DNN filter, the limit of detection (LOD) of methane was 86.62 ppb with an average time of 1 s, decreasing to 12.03 ppb with an average time of 229 s, which is a significant promotion compared to similar work reported. The high sensitivity and stability of the proposed sensor are shown through a 24-hour continuous monitoring experiment of atmospheric methane conducted outdoors, providing a new solution for high-sensitivity remote sensing of atmospheric methane.

Graphene oxide: Synthesis and laser spectroscopy approach

Nanotechnology research offers advancements in materials and industrial uses such as nano-electronics, medical sciences, fuel, biology, and technological innovation. The most often employed nanomaterial is Graphene oxide (GO), which has been regarded as a dominant progenitor for many specialized industries. The current work aims to establish a new, cost-effective, easy, and straightforward GO synthesis method. Laser spectroscopy and even traditional tools have been utilized for characterization. The prepared GO has been confirmed by XRD and FT-IR spectroscopy. Laser spectroscopy based on confocal microscopes like Raman micro-spectroscopy and fluorescence lifetime imaging microscopy (FLIM) has been used to ensure the synthesis of GO. Also, it could help in the detection of the prepared layer thickness. Raman spectroscopy detects the number of GO layers, which is one on average, while the Raman mapping shows a good distribution of GO on the substrate. Based on excitation with a 445 nm pulsed laser, FLIM shows that mono GO layers cover most of the surface while only a tiny area contains more than a single layer. The novel aspect of this work is the method of preparation and the way of utilizing both FLIM and Raman to detect the number of GO layers. The prepared GO could be used in many applications like solar cells and filtration.

Lunar Flashlight science ground and flight measurements and operations using a multi-band laser reflectometer

The Lunar Flashlight cubesat mission was designed and flown to collect new data on the abundance and distribution of water ice frost in lunar permanently shadowed regions (PSRs) using active laser spectroscopy. Key advantages of active spectroscopy are that it can collect surface reflectance data in locations and conditions where passive spectroscopy cannot operate, specifically nightside locations where no indirect lighting is available, and in the deepest parts of PSRs where indirect lighting may be too faint for passive spectroscopy. Lunar Flashlight launched in 2022 but because of a propulsion system failure, did not make it to the Moon to conduct its science investigation. However, Lunar Flashlight proved to be an extremely successful technology demonstration mission, meeting or exceeding all its technology-focused mission goals, including demonstrating its instrument functionality. This paper describes the extensive ground and test campaigns to characterize the Lunar Flashlight laser reflectometer instrument and its planned utility for science observations, along with recommendations for future instrument design, development, verification, and use.

Measurement of Light-Duty Vehicle Exhaust Emissions with Light Absorption Spectrometers

Light-duty vehicle emission regulations worldwide set limits for the following gaseous pollutants: carbon monoxide (CO), nitric oxides (NOX), hydrocarbons (HCs), and/or non-methane hydrocarbons (NMHCs). Carbon dioxide (CO2) is indirectly limited by fleet CO2 or fuel consumption targets. Measurements are carried out at the dilution tunnel with “standard” laboratory-grade instruments following well-defined principles of operation: non-dispersive infrared (NDIR) analyzers for CO and CO2, flame ionization detectors (FIDs) for hydrocarbons, and chemiluminescence analyzers (CLAs) or non-dispersive ultraviolet detectors (NDUVs) for NOX. In the United States in 2012 and in China in 2020, with Stage 6, nitrous oxide (N2O) was also included. Brazil is phasing in NH3 in its regulation. Alternative instruments that can measure some or all these pollutants include Fourier transform infrared (FTIR)- and laser absorption spectroscopy (LAS)-based instruments. In the second category, quantum cascade laser (QCL) spectroscopy in the mid-infrared area or laser diode spectroscopy (LDS) in the near-infrared area, such as tunable diode laser absorption spectroscopy (TDLAS), are included. According to current regulations and technical specifications, NH3 is the only component that has to be measured at the tailpipe to avoid ammonia losses due to its hydrophilic properties and adsorption on the transfer lines. There are not many studies that have evaluated such instruments, in particular those for “non-regulated” worldwide pollutants. For this reason, we compared laboratory-grade “standard” analyzers with FTIR- and TDLAS-based instruments measuring NH3. One diesel and two gasoline vehicles at different ambient temperatures and with different test cycles produced emissions in a wide range. In general, the agreement among the instruments was very good (in most cases, within ±10%), confirming their suitability for the measurement of pollutants.

Towards Precision Muonic X-ray Measurements of Charge Radii of Light Nuclei

We, the QUARTET Collaboration, propose an experiment to measure the nuclear charge radii of light elements with up to 20 times higher accuracy. These are essential both for understanding nuclear physics at low energies, and for experimental and theoretical applications in simple atomic systems. Such comparisons advance the understanding of bound-state quantum electrodynamics and are useful for searching for new physics beyond the Standard Model. The energy levels of muonic atoms are highly susceptible to nuclear structure, especially to the mean square charge radius. The radii of the lightest nuclei (with the atomic number, Z=1,2) have been determined with high accuracy using laser spectroscopy in muonic atoms, while those of medium mass and above were determined using X-ray spectroscopy with semiconductor detectors. In this communication, we present a new experiment, aiming to obtain precision measurements of the radii of light nuclei 3≤Z≤10 using single-photon energy measurements with cryogenic microcalorimeters; a quantum-sensing technology capable of high efficiency with outstanding resolution for low-energy X-rays.

Zero-Quantum-Defect Method and the Fundamental Vibrational Interval of H_{2}^{+}.

The fundamental vibrational interval of H_{2}^{+} has been determined to be ΔG_{1/2}=2191.126 614(17) cm^{-1} by continuous-wave laser spectroscopy of Stark manifolds of Rydberg states of H_{2} with the H_{2}^{+} ion core in the ground and first vibrationally excited states. Extrapolation of the Stark shifts to zero field yields the zero-quantum-defect positions -R_{H_{2}}/n^{2}, from which ionization energies can be determined. Our new result represents a 4-order-of-magnitude improvement compared to earlier measurements. It agrees, within the experimental uncertainty, with the value of 2191.126 626 344(17)(100) cm^{-1} determined in nonrelativistic quantum electrodynamic calculations [V. Korobov, L. Hilico and J.-Ph. Karr, Phys. Rev. Lett. 118, 233001 (2017)PRLTAO0031-900710.1103/PhysRevLett.118.233001].

Online Testing Method for the Fine Spectral Characteristics of Narrow-Band Interference Filters Based on a Narrow-Linewidth Tunable Laser.

The transmission spectrum of a narrow-band interference filter is crucial and highly influenced by factors such as the temperature and angle, thus requiring precise and online measurements. The traditional method of measuring the transmission spectrum of an interference filter involves the use of a spectrometer, but the accuracy of this method is limited. Moreover, placing a narrow-band interference filter inside a spectrometer hinders real-time online measurements. To address this issue, there is demand for high-precision online spectral testing methods. In response to this demand, we propose and experimentally validate a fine spectral characterization method for narrow-band interference filters. This method uses a narrow-linewidth tunable laser, achieving a spectral resolution in the MHz range for online testing. Two types of narrow-band interference filters were tested using the constructed laser spectroscopy experimental system, obtaining a transmission spectrum with a spectral resolution of 318 MHz. In comparison to spectrometer-based methods, our proposed method demonstrates higher spectral accuracy, enables online measurements, and provides more accurate measurements for special spectral interference filters. This approach has significant application value and promising development prospects.

Carbon Monoxide Dissociation at Planetary Entry Conditions Examined by Megahertz-Rate Laser Spectroscopy

A study of carbon monoxide (CO) dissociation was performed in a shock tube at conditions relevant to the high-speed entry of Venus and Mars atmospheres. The CO number density (or mole fraction) and the temperature are probed behind reflected shock waves at 1 MHz using scanned-wavelength laser absorption spectroscopy near 2011 cm−1 (4.97 μm). The wide range of vibrational states (v=1, 4, 8, and 10) probed by this technique enables precise number density and temperature measurements up to and above 9000 K using a Boltzmann population fit of the resolved spectral lines. Mixtures of CO diluted in Ar at 3–60% are shock-heated in a wide range of conditions (T5=4650−11,150 K at p5=0.26–4.07 atm) and compared to state-of-the-art chemical kinetic models. The time-resolved measurements of temperature and number density behind reflected shock waves are utilized to infer the rate coefficients of CO+M→C+O+M for M=CO, Ar. They are found to be kdiss,CO=1.8×1028⋅T−2.7exp(−129,000/T) cm3/(mol⋅s) and kdiss,Ar=1.5×1025⋅T−2.1exp(−129,000/T) cm3/(mol⋅s).

Stable, intense supercontinuum light generation at 1 kHz by electric field assisted femtosecond laser filamentation in air

Supercontinuum (SC) light source has advanced ultrafast laser spectroscopy in condensed matter science, biology, physics, and chemistry. Compared to the frequently used photonic crystal fibers and bulk materials, femtosecond laser filamentation in gases is damage-immune for supercontinuum generation. A bottleneck problem is the strong jitters from filament induced self-heating at kHz repetition rate level. We demonstrated stable kHz supercontinuum generation directly in air with multiple mJ level pulse energy. This was achieved by applying an external DC electric field to the air plasma filament. Beam pointing jitters of the 1 kHz air filament induced SC light were reduced by more than 2 fold. The stabilized high repetition rate laser filament offers the opportunity for stable intense SC generation and its applications in air.

Hard-Target Reflection Laser Spectroscopy of Carbon Monoxide Gas Concentration for the Early Detection of Spontaneous Combustion of Coal.

We report on the hard-target reflection spectroscopy of carbon monoxide (CO) gas based on the technique of infrared tunable diode laser absorption spectroscopy aiming at developing a low-cost yet sensitive sensor for the early detection of spontaneous coal combustion. A narrow-band distributed feedback laser emitting around 2333.7 nm is used to monitor CO gas molecules contained in a 5 cm gas cell. The light diffusely backscattered from the surface of a lump of coal placed at the end of a 50 cm light path is detected with a photodiode in the coaxial transmitter/receiver setup. From the variation of the detected signal profile with the CO partial pressure in the cell, the detection limit of the current system is estimated to be about 30 parts per million per meter (ppm·m), which meets the sensitivity required for monitoring the self-heating of coal in mines, silos, or stockpiles.

Nuclear structure studies by collinear laser spectroscopy

Nuclear structure studies by collinear laser spectroscopy