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Data supporting manuscript submitted to PNAS: Video-Rate Raman-based Metabolic Imaging by Airy Light-Sheet Illumination and Photon-Sparse Detection. The data set includes: [1] raw data and [2] related images used in the analyses described within the manuscript.
Raman spectra of Na 2 Ca 2 (CO 3 ) 3 shortite and K 2 Ca(CO 3 ) 2 bütschliite were measured to 715°C and 740°C respectively, under vacuum. The vibrational spectra demonstrate that shortite converts to nyerereite (Na 2 Ca(CO 3 ) 2 ) and calcite at 535°C. This assemblage is stable to ~700°C, where nyerereite begins to decompose. Bütschliite converts to the isochemical phase fairchildite at 570°C, which is stable to 665°C, where it decomposes to an assemblage of K 2 CO 3 and CaO. The variation of anharmonicity between different vibrational modes of each of the low temperature phases is assessed, and these yield insights into inter-carbonate group couplings. In conclusion, both fairchildite and nyerereite exhibit spectral features consistent with extensive disordering.
Raman spectroscopy is currently used at SRNL to measure the concentration of gaseous species evolved from chemical reactions. This report documents the methods used to calibrate the spectroscopic systems in both frequency and intensity spaces.
This final technical report details the accomplishment and findings of a project that developed technology related to imaging metabolic processes in plants. The report gives technical details of the design, construction and characterization of a Raman microscope system capable of identifying chemical species using the wavelength shifts of scattered excitation light. Some of the unique aspects of the design include: use of a Bessel beam excitation source, which allow long excitation lines that are resistant to scattering in complex media such as plants; excitation at 785 nm to avoid fluorescence emission that can occur in photosynthetic organisms; and a flat optical design that makes construction and alignment significantly simpler. This project also used stable isotope labeling to look at photorespiratory flux in the leaves of three different types of plants that have different photosynthesis pathways. Gas chromatography–mass spectrometry was used to look at which metabolites and amino acids had altered oxygen, carbon and hydrogen uptake under various conditions of environmental oxygen. This generated a rich data set that is being further analyzed to understand metabolic pathways in plants. This project also used the natural fluorescence in sorghum and rice to conduct an extensive experiment across different developmental stages. Spectral differences were identified at most of the developmental stages and these can be attributed to differential pigment and pigment-protein complexes present in different relative abundances as the plant develops.
In April 2022 the National Urban Security Technology Laboratory’s System Assessment and Validation for Emergency Responders program conducted an operational assessment of ten commercially available handheld Raman spectrometers. Additionally, prior to the operational assessment, the Pacific Northwest National Laboratory conducted laboratory testing of the devices, including scanning a number of samples in various containers. This report summarizes the results of the assessment.
Fibromyalgia (FM) is a chronic muscle pain disorder that shares several clinical features with other related rheumatologic disorders. This study investigates the feasibility of using surface-enhanced Raman spectroscopy (SERS) with gold nanoparticles (AuNPs) as a fingerprinting approach to diagnose FM and other rheumatic diseases such as rheumatoid arthritis (RA), systemic lupus erythematosus (SLE), osteoarthritis (OA), and chronic low back pain (CLBP). Blood samples were obtained on protein saver cards from FM (n = 83), non-FM (n = 54), and healthy (NC, n = 9) subjects. A semi-permeable membrane filtration method was used to obtain low-molecular-weight fraction (LMF) serum of the blood samples. SERS measurement conditions were standardized to enhance the LMF signal. An OPLS-DA algorithm created using the spectral region 750 to 1720 cm -1 enabled the classification of the spectra into their corresponding FM and non-FM classes (Rcv > 0.99) with 100% accuracy, sensitivity, and specificity. The OPLS-DA regression plot indicated that spectral regions associated with amino acids were responsible for discrimination patterns and can be potentially used as spectral biomarkers to differentiate FM and other rheumatic diseases. This exploratory work suggests that the AuNP SERS method in combination with OPLS-DA analysis has great potential for the label-free diagnosis of FM.
The equation of state and stability of topaz at high-pressure/high-temperature conditions have been investigated by in situ synchrotron X-ray diffraction (XRD) and Raman spectroscopy in this study. No phase transition occurs on topaz over the experimental pressure–temperature ($P-T$) range. The pressure–volume data were fitted by the third-order Birch–Murnaghan equation of state (EoS) with the zero-pressure unit–cell volume V 0 = 343.86 (9) Å 3 , the zero-pressure bulk modulus K 0 = 172 (3) GPa, and its pressure derivative K’ 0 = 1.3 (4), while the obtained K 0 = 155 (2) GPa when fixed K’ 0 = 4. In the pressure range of 0–24.4 GPa, the vibration modes of in-plane bending OH-groups for topaz show non-linear changes with the increase in pressure, while the other vibration modes show linear changes. Moreover, the temperature–volume data were fitted by Fei’s thermal equation with the thermal expansion coefficient α 300 = 1.9 (1) × 10 –5 K –1 at 300 K. Finally, the $P-T$ stability of topaz was studied by a synchrotron-based single-crystal XRD at simultaneously high $P-T$ conditions up to ~10.9 GPa and 700 K, which shows that topaz may maintain a metastable state at depths above 370 km in the upper mantle along the coldest subducting slab geotherm. Thus, topaz may be a potential volatile-carrier in the cold subduction zone. It can carry hydrogen and fluorine elements into the deep upper mantle and further affect the geochemical behavior of the upper mantle.
The ice cloud detection sensitivity of the millimeter cloud radar (MMCR) and the Ka-band Zenith radar (KAZR) is investigated using a collocated Raman lidar (RL) at the Atmospheric Radiation Measurement Program Southern Great Plains site. Only profiles that are transparent to the RL with ice clouds only are considered in this study. The MMCR underestimates the RL ice cloud optical depth (COD) by 20%. The MMCR detects no ice clouds in 37% of the profiles. These profiles where ice cloud goes undetected by the MMCR typically contain very optically thin clouds, with a mean RL ice COD of 0.03. Higher ice cloud detection sensitivity is found for the KAZR, which underestimates the RL ice COD by 15%. The decrease in the ice COD bias for the KAZR compared to the MMCR is largely due to a decrease in the ice COD bias for the situation where the transparent profiles with ice clouds are detected by both the RL and cloud radar. The climatic net ice cloud radiative effects (CREs) from the RL at the top of the atmosphere (TOA) and the surface are 3.2 W m−2 and −0.6 W m−2, respectively. The ice CREs at the TOA and surface are underestimated for the MMCR by 0.7 W m−2 and 0.16 W m−2 (21% and 29%) and underestimated for the KAZR by 0.6 W m−2 and 0.14 W m−2 (17% and 24%). The ice clouds undetected by the cloud radars led to underestimating the climatic net cloud heating rates below 150 hPa by about 0–0.04 K day−1.
The Karlsruhe Tritium Neutrino (KATRIN) experiment aims at measuring the effective electron neutrino mass with a sensitivity of 0.2 eV/c2, i.e., improving on previous measurements by an order of magnitude. Neutrino mass data taking with KATRIN commenced in early 2019, and after only a few weeks of data recording, analysis of these data showed the success of KATRIN, improving on the known neutrino mass limit by a factor of about two. This success very much could be ascribed to the fact that most of the system components met, or even surpassed, the required specifications during long-term operation. Here, we report on the performance of the laser Raman (LARA) monitoring system which provides continuous high-precision information on the gas composition injected into the experiment’s windowless gaseous tritium source (WGTS), specifically on its isotopic purity of tritium—one of the key parameters required in the derivation of the electron neutrino mass. The concentrations cx for all six hydrogen isotopologues were monitored simultaneously, with a measurement precision for individual components of the order 10−3 or better throughout the complete KATRIN data taking campaigns to date. From these, the tritium purity, εT, is derived with precision of <10−3 and trueness of <3 × 10−3, being within and surpassing the actual requirements for KATRIN, respectively.
The planetary boundary layer (PBL) plays a critical role in the atmosphere by transferring heat, moisture, and momentum. The warm PBL has a distinct diurnal cycle including the daytime convective mixing layer (ML) and nighttime residual layer developments. Thus, simultaneous determinations of PBL height (PBLH) and ML height (MLH) are necessary for studying PBL characterization and processes. Here, new approaches are developed to provide reliable PBLH and MLH estimates to characterize warm PBL evolution. The approaches use Raman lidar (RL) water vapor mixing ratio (WVMR) and Doppler lidar (DL) vertical velocity measurements at the Southern Great Plains (SGP) atmospheric observatory, which was established by the Atmospheric Radiation Measurement (ARM) User Facility. Compared to widely used lidar aerosol measurements for PBLH, WVMR is a better tracer for PBL vertical mixing. For PBLH, the approach classifies PBL water vapor structures into a few general patterns, then uses a slope method and dynamic threshold method to determine PBLH. For MLH, wavelet analysis is used to reconstruct 2D variance from DL vertical wind velocity measurements according to the turbulence eddy size to minimize the impacts of gravity wave and eddy size on variance calculations; then, a dynamic threshold method is used to determine MLH. Remotely-sensed PBLHs and MLHs are compared with radiosonde measurements based on the Richardson number method. Good agreements between them confirm that the proposed new algorithms are reliable for PBLH and MLH characterization. The algorithms are applied to warm-season RL and ML measurements at the SGP site for five years to study warm-season PBL structure and processes. The weekly composited diurnal evolutions of PBLHs and MLHs in a warm climate were provided to illustrate diurnal and seasonal PBL evolutions. This reliable data set of PBLH and MLH values will be valuable for studying PBL processes, model evolution, and PBL parameterization improvements. The MLH dataset includes the MLH in values of km above ground level. The PBLH dataset includes the PBLH in values of km above ground level, along with a flag ("situation_PBLH") to determine the state of the PBL (1 = Cloudy Condition, 2 = Stable Layer, 3 = Multi-layer WVMR structure, 4 = Well-Mixed PBL, 5 = A de-coupled layer, 6 = Other).
Angular emission properties of stimulated Raman radiation from liquids, noting two classes of radiation
Two-phonon Raman scattering in cubic crystals, noting use of polarization effect to determine active irreducible representations
Vibrational spectrum of liquid, solid and gaseous tetradeuterated hydrazine and Raman study of hydrogen bonding in hydrazine
Calculation method for true profile of Raman lines
Stimulated Raman effects in anisotropic crystal potassium dihydrogen phosphate with Stokes generations
Electric field enhanced Raman scattering and linear frequency shift of strontium titanate soft mode in random domain orientation and reorientation
Stimulated Raman scattering in IR active nontotally symmetric vibration of alpha quartz crystal, noting parametric oscillation
We have elecited a reliable glucose signature in mammalian physiological ranges using near infrared Raman laser excitation at 785 nm and multivariate analysis. In a recent series of experiments we measured glucose levels in an artificial aqueous humor in the range from 0.5 to 13X normal values.