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Stratospheric measurements possible with ground-based, airborne, and satellite-borne lidar systems are reviewed. The instruments, basic equations, and formats normally used for various scattering and absorption phenomena measurements are presented including a discussion of elastic, resonance, Raman, and fluorescence scattering techniques.
This paper reviews stratospheric measurements possible with ground-based, airborne, and satellite-borne lidar systems. The instruments, basic equations, and formats normally used for various scattering and absorption phenomena measurements are presented including a discussion of elastic, resonance, Raman, and fluorescence scattering techniques.
Molecular rotations and kinetics from spectral features of molecular Raman spectra, using light scattering spectroscopy
An approach is described for measuring hydration-induced volume change within ion conductive polymer membranes and thin films by adapting the technique of confocal Raman microscopy. With careful consideration of factors that affect excitation and scattering within the confocal probe volume region, material swelling and deswelling were estimated from the intensities of polymer matrix spectral features. A high numerical aperture oil-immersion objective was used to achieve tight focusing within samples and the efficient collection of Raman scattered light. The approach is demonstrated for a fluorinated cation-exchange ionomer (Nafion) and the hydrocarbon anion-exchange ionomer Sustainion. Samples were monitored while under a nitrogen atmosphere that was cycled between dry and humid (∼50% relative humidity, RH) states. The volume changes estimated from the Raman spectra were in close agreement with those derived from conventional measurements. The reported work advances understanding needed to adapt confocal Raman microscopy for quantitative in situ and operando studies of ionomers within electrochemical devices, such as polymer electrolyte membrane fuel cells and electrolyzers, and lays a foundation for broader applications in the study of hydration-induced polymer swelling and the associated molecular level water and polymer framework structural changes.
Multimaterial and Isotopically Labeled Specimen Fabrication via Material Extrusion Additive Manufacturing for Interlayer Diffusion Analysis
An innovative solution for real-time monitoring of reactions within confined spaces, optimized for Raman spectroscopy applications, is presented. This approach involves the utilization of a hollow-core waveguide configured as a compact flow cell, serving both as a conduit for Raman excitation and scattering and seamlessly integrating into the effluent stream of a cracking catalytic reactor. The analytical technique, encompassing device and optical design, ensures robustness, compactness, and cost-effectiveness for implementation into process facilities. Notably, the modularity of the approach empowers customization for diverse gas monitoring needs, as it readily adapts to the specific requirements of various sensing scenarios. As a proof of concept, the efficacy of a spectroscopic approach is shown by monitoring two catalytic processes: CO 2 methanation (CO 2 + 4H 2 → CH 4 + 2H 2 O) and ammonia cracking (2NH 3 → N 2 + 3H 2 ). Leveraging chemometric data processing techniques, spectral signatures of the individual components involved in these reactions are effectively disentangled and the results are compared to mass spectrometry data. This robust methodology underscores the versatility and reliability of this monitoring system in complex chemical environments.
In highly concentrated electrolyte solutions, where classical models often fail, specific ion–solvent interactions dictate bulk properties. Here, in this study, we combine small-angle X-ray scattering (SAXS) and Raman spectroscopy to link molecular coordination to mesoscale structure across alkali nitrate and nitrite solutions. Our results reveal a structural hierarchy driven by cation identity in that smaller cations (Li + , Na + ) form discrete contact ion pairs, while larger cations (K + , Rb + ) promote increasingly disordered local coordination and extended solute–solvent networks. Using nitrite salts as a structural control, we confirm this organizing principle across different anion geometries. Cs + undergoes a concentration-induced transition to a uniquely ordered state, resulting in a highly structured solution. This work provides a direct, mechanistic explanation for how cation choice dictates the ‘rules’ of solution architecture, offering a predictive basis for understanding phase behavior in complex industrial and environmental systems.
This paper discusses the application of lidar (laser radar) to the measurement of air pollution. Lidar techniques and instrumentation utilizing elastic, Raman, and fluorescence scattering are discussed. Data showing measurements of the mixing of particulate pollutants in the atmosphere are presented. These data include: simultaneous two-wavelength results, isopleths showing the temporal dynamics of particulate mixing, measurements of the top of the earth's mixing layer, and measurements in a valley with restricted circulation and mixing. All measurements are compared with simultaneous radiosonde and/or aircraft-mounted temperature probe support. In addition, a second generation lidar system presently under development is described.
A bibliography is given of 1460 references of the applications of lasers to atmospheric sciences. The subjects covered include: aerosols; clouds; the distribution and motion of atmospheric natural and man-made constituents; winds; temperature; turbulence; scintillation; elastic, Raman and resonance scattering; fluorescence; absorption and transmission; the application of the Doppler effect and visibility. Instrumentation, in particular lidar, is included, also data handling, and interpretation of the data for meteorological processes. Communications, geodesy and rangefinding are not included as distinct areas. The application to the atmosphere is covered, but not the ocean or its surface.
A method is described in which a pulsed laser is used to probe the sea. Backscattered light is analyzed in time, intensity and wavelength. Tyndall, Raman and Brillouin scattering are used to obtain the backscatter turbidity, sound velocity, salinity, and the temperature as a function of depth.
The application of pulsed resonance spectroscopy to the measurement of species concentrations in chemically reacting turbulent flows is discussed. The theory of such measurements is developed. An uncertainty analysis is performed, and the results are applied to typical combustion conditions. Experimental aspects are discussed. The method shows a significant theoretical improvement in accuracy over Raman and Reyleigh scattering techniques, and no significant barriers appear to block its development.
Protein crystals are so fragile that they often can not be handled by tweezers. Indeed, measurements of the Young modulus, E, of lysozyme crystals resulted in E approx. equals 0.1 - 1 GPa, the lower figures, 0.1 - 0.5 GPa, being obtained from triple point bending of as-grown and not cross-linked crystals sitting in solution. The bending strength was found to be approx.10(exp -2) E. On the other hand, ultrasound speed and Mandelstam-Raman-Brilloin light scattering experiments led to much higher figures, E approx. equals 2.7 GPa. The lower figures for E were found from static or low frequency crystal deformations measurements, while the higher moduli are based on high frequency lattice vibrations, 10(exp 7) - 10(exp 10) 1/s. The physical reason for the about an order of magnitude discrepancy is in different behavior of water filling space between protein molecules. At slow lattice deformation, the not-bound intermolecular water has enough time to flow from the compressed to expanded regions of the deformed crystal. At high deformation frequencies in the ultra- and hypersound waves, the water is confined in the intermolecular space and, on that scale, behaves like a solid, thus contributing to the elastic crystal moduli. In this case, the reciprocal crystal modulus is expected to be an average of the water protein and water compressibilities (reciprocal compressibilities): the bulk modulus for lysozyme is 26 GPa, for water it is 7 GPa. Anisotropy of the crystal moduli comes from intermolecular contacts within the lattice while the high frequency hardness comes from the bulk of protein molecules and water bulk moduli. These conclusions are based on the analysis of liquid flow in porous medium to be presented.
Engineers charged with making jet aircraft quieter have long dreamed of being able to see exactly how turbulent eddies produce sound and this dream is now coming true with the advent of large eddy simulation (LES). Two obvious challenges remain: validating the LES codes at the resolution required to see the fluid-acoustic coupling, and the interpretation of the massive datasets that result in having dreams come true. This paper primarily addresses the former, the use of advanced experimental techniques such as particle image velocimetry (PIV) and Raman and Rayleigh scattering, to validate the computer codes and procedures used to create LES solutions. It also addresses the latter problem in discussing what are relevant measures critical for aeroacoustics that should be used in validating LES codes. These new diagnostic techniques deliver measurements and flow statistics of increasing sophistication and capability, but what of their accuracy? And what are the measures to be used in validation? This paper argues that the issue of accuracy be addressed by cross-facility and cross-disciplinary examination of modern datasets along with increased reporting of internal quality checks in PIV analysis. Further, it is argued that the appropriate validation metrics for aeroacoustic applications are increasingly complicated statistics that have been shown in aeroacoustic theory to be critical to flow-generated sound.
Engineers charged with making jet aircraft quieter have long dreamed of being able to see exactly how turbulent eddies produce sound and this dream is now coming true with the advent of large eddy simulation (LES). Two obvious challenges remain: validating the LES codes at the resolution required to see the fluid-acoustic coupling, and the interpretation of the massive datasets that are produced. This paper addresses the former, the use of advanced experimental techniques such as particle image velocimetry (PIV) and Raman and Rayleigh scattering, to validate the computer codes and procedures used to create LES solutions. This paper argues that the issue of accuracy of the experimental measurements be addressed by cross-facility and cross-disciplinary examination of modern datasets along with increased reporting of internal quality checks in PIV analysis. Further, it argues that the appropriate validation metrics for aeroacoustic applications are increasingly complicated statistics that have been shown in aeroacoustic theory to be critical to flow-generated sound, such as two-point space-time velocity correlations. A brief review of data sources available is presented along with examples illustrating cross-facility and internal quality checks required of the data before it should be accepted for validation of LES.
Since the eruption of Mt. Pinatubo in June, 1991, measurements of atmospheric species which depend on Rayleigh scattering of radiation, have been severely compromised where the volcanic aerosol cloud exists. For the GSFC stratospheric ozone lidar, this has meant that ozone determination has been impossible below approximately 30 km. The GSFC lidar has been modified to detect Raman scattering from nitrogen molecules from transmitted laser wavelengths. The instrument transmits two laser wavelengths at 308 nm and 351 nm, and detects returns at four wavelengths; 308 nm, 332 nm, 351 nm, and 382 nm. Using this technique in conjunction with the Rayleigh DIAL measurement, ozone profiles have been measured between 15 and 50 km.
This paper describes the characterization of a combined Coherent anti-Stokes Raman Spectroscopy and Interferometric Rayleigh Scattering (CARS-IRS) system by reporting the accuracy and precision of the measurements of temperature, species mole fraction of N2, O2, and H2, and two-components of velocity. A near-adiabatic H2-air Hencken burner flame was used to provide known properties for measurements made with the system. The measurement system is also demonstrated in a small-scale Mach 1.6 H2-air combustion-heated supersonic jet with a co-flow of H2. The system is found to have a precision that is sufficient to resolve fluctuations of flow properties in the mixing layer of the jet.
This study investigates the solvation structures and dynamics of bis(trifluoromethanesulfonyl)imide (TFSI – )-based aqueous electrolytes, focusing on Fe(TFSI) 2 and Fe(TFSI) 3 . Using advanced characterization techniques, including small-angle X-ray scattering, molecular dynamics simulations, Raman spectroscopy, Fourier-transform infrared spectroscopy, and nuclear magnetic resonance, we elucidate how the electrolyte concentration influences ion association, solvation structures, and transport properties. Furthermore, our findings show that higher electrolyte concentrations promote the formation of contact ion pairs and anion networks, leading to reduced ion mobility and altered hydrogen-bonding dynamics. These insights provide a deeper understanding of solvation phenomena in TFSI-based electrolytes and contribute to the development of efficient and environmentally friendly iron electrodeposition processes.
Chemical transformations near plasmonic metals have attracted increasing attention in the past few years. Specifically, reactions occurring within plasmonic nanojunctions that can be detected via surface and tip-enhanced Raman (SER and TER) scattering were the focus of numerous reports. In this context, even though the transition between localized and nonlocal (quantum) plasmons at nanojunctions is documented, its implications on plasmonic chemistry remain poorly understood. We explore the latter through AFM-TER-current measurements. We use two molecules: i) 4-mercaptobenzonitrile (MBN) that reports on the (non)local fields and ii) 4-nitrothiophenol (NTP) that features defined signatures of its neutral/anionic forms and dimer product, 4,4′-dimercaptoazobenzene (DMAB). The transition from classical to quantum plasmons is established through our optical measurements: It is marked by molecular charging and optical rectification. Simultaneously recorded force and current measurements support our assignments. In the case of NTP, we observe the parent and DMAB product beneath the probe in the classical regime. Further reducing the gap leads to the collapse of DMAB to form NTP anions. The process is reversible: Anions subsequently recombine into DMAB. Our results have significant implications for AFM-based TER measurements and their analysis, beyond the scope of this work. In effect, when precise control over the junction is not possible (e.g., in SER and ambient TER), both classical and quantum plasmons need to be considered in the analysis of plasmonic reactions