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At least 757 records · Page 42
All sourcesNASA NTRSDOE OSTI
DOE OSTI2015

Drought onset mechanisms revealed by satellite solar-induced chlorophyll fluorescence: Insights from two contrasting extreme events

This study uses the droughts of 2011 in Texas and 2012 over the central Great Plains as case studies to explore the potential of satellite-observed solar-induced chlorophyll fluorescence (SIF) for monitoring drought dynamics. We find that the spatial patterns of negative SIF anomalies from the Global Ozone Monitoring Experiment 2 (GOME-2) closely resembled drought intensity maps from the U.S. Drought Monitor for both events. The drought-induced suppression of SIF occurred throughout 2011 but was exacerbated in summer in the Texas drought. This event was characterized by a persistent depletion of root zone soil moisture caused by yearlong below-normal precipitation. In contrast, for the central Great Plains drought, warmer temperatures and relatively normal precipitation boosted SIF in the spring of 2012; however, a sudden drop in precipitation coupled with unusually high temperatures rapidly depleted soil moisture through evapotranspiration, leading to a rapid onset of drought in early summer. Accordingly, SIF reversed from above to below normal. For both regions, the GOME-2 SIF anomalies were significantly correlated with those of root zone soil moisture, indicating that the former can potentially be used as proxy of the latter for monitoring agricultural droughts with different onset mechanisms. Further analyses indicate that the contrasting dynamics of SIF during these two extreme events were caused by changes in both fraction of absorbed photosynthetically active radiation fPAR and fluorescence yield, suggesting that satellite SIF is sensitive to both structural and physiological/biochemical variations of vegetation. Here, we conclude that the emerging satellite SIF has excellent potential for dynamic drought monitoring.

58 GEOSCIENCES↗
DOE OSTI2018

Annihilation Delayed Fluorescence of Indole and Its Derivatives in Aqueous Solution

Spectral and kinetic characteristics of annihilation delayed fluorescence (ADF) of indole and its derivatives (5-methylindole, N-methylindole) were measured in aqueous solutions at room temperature. ADF spectra of indole and 5-methylindole consisted of two bands with wavelength maxima at 350 and 425 nm for indole and 350 and 390 nm for 5-methylindole. The short-wavelength band was due to ADF of monomers and coincided with the fast fluorescence spectrum. The long-wavelength band was attributed to ADF of excimers, the excited singlet states of which were populated by annihilation of triplet excimers. Triplet states of excimers were formed by collisions of molecules in triplet and ground states. The ADF spectrum of N-methylindole consisted of only the short-wavelength ADF band of monomers (λ = 352 nm). Lifetimes of monomer and excimer triplet states were estimated from the ADF kinetics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2018

Taking into Account Interelement Interference in X-Ray Fluorescence Analysis of Thin Two-Layer Ti/V Systems

We propose a new method for determining the thickness of layers in x-ray fluorescence analysis of two-layer Ti/V systems, using easily fabricated standardized film layers obtained by sputter deposition of titanium on a polymer film substrate. We have calculated correction factors taking into account the level of attenuation for the intensity of the primary emission from the x-ray tube and the analytical line for the element of the bottom layer in the top layer, and the enhancement of the fluorescence intensity for the top layer by the emission of atoms in the bottom layer.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2018

Early Stage Detection of Stress Due to Copper on Maize (Zea mays L.) by Laser-Induced Fluorescence and Infrared Spectroscopy

Laser-induced fluorescence (LIF) and attenuated total reflectance Fourier transform infrared (ATR-FTIR) spectroscopy has been applied for the nondestructive, label free, and rapid analyses of the impact of copper (25, 50, and 75 μM) on maize seedlings at an early stage before the changes appear visually on the plant. The LIF measurement has been used to detect the signs of stress in the photosynthetic pigment. The integrated areal intensity and increasing fluorescence intensity ratios indicate decrease in the photosynthetic pigments in the leaves of maize plants stressed with copper. The ATR-FTIR technique has been utilized to estimate the changes arising in the cell wall polysaccharides, amino acid, secondary structure of protein and lipid content of the leaves of control and copper-treated maize seedlings. The second derivative and curve fitting analyses have been applied for the enhancement of the spectral variations and quantitative estimation of the changes arising in the biochemical profile. The result shows an increase in the pectin, lignin, amino acid, and protein content and reduction in the amount of cellulose and lipid in the leaves of maize seedlings due to the treatment of copper. This study indicates the toxic response of copper by hampering the growth and reduction in the photosynthetic pigments and biochemical content of the maize seedlings. This study also demonstrates the feasibility of the spectroscopic techniques (LIF and ATRFTIR) as a rapid, label free, and nondestructive probe for the assessment of stress and monitoring of crops.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Investigation of Molecular Diffusion at Block Copolymer Thin Films Using Maximum Entropy Method-Based Fluorescence Correlation Spectroscopy and Single Molecule Tracking

Fluorescence correlation spectroscopy (FCS) has been widely used to investigate molecular diffusion behavior in various samples. The use of the maximum entropy method (MEM) for FCS data analysis provides a unique means to determine multiple distinct diffusion coefficients without a priori assumption of their number. Comparison of the MEM-based FCS method (MEM-FCS) with another method will reveal its utility and advantage as an analytical tool to investigate diffusion dynamics. Herein, we measured diffusion of fluorescent probes doped into nanostructured thin films using MEM-FCS, and validated the results with single molecule tracking (SMT) data. The efficacy of the MEM code employed was first demonstrated by analyzing simulated FCS data for systems incorporating one and two diffusion modes with broadly distributed diffusion coefficients. The MEM analysis accurately afforded the number of distinct diffusion modes and their mean diffusion coefficients. These results contrasted with those obtained by fitting the simulated data to conventional two-component and anomalous diffusion models, which yielded inaccurate estimates of the diffusion coefficients. Subsequently, the MEM analysis was applied to FCS data acquired from hydrophilic dye molecules incorporated into microphase-separated polystyrene-block-poly(ethylene oxide) (PS-b-PEO) thin films characterized under a water-saturated nitrogen atmosphere. The MEM analysis revealed distinct fast and slow diffusion components attributable to molecules diffusing on the film surface and inside the film, respectively. SMT studies of the same materials yielded trajectories for mobile molecules that appear to follow the curved PEO microdomains. Diffusion coefficients obtained from the SMT data were consistent with those obtained for the slow diffusion component detected by MEM-FCS. Furthermore, these results highlight the utility of MEM-FCS and SMT for gaining complementary information on molecular diffusion processes in heterogeneous material systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Control of optical absorption and fluorescence spectroscopies of natural melanin at different solution concentrations

The source of the optical properties of natural melanin persists as an impressive conundrum, hindering a thorough comprehension of the complicated photo-protective contribution of these extensive natural pigments and the pragmatic design of revolutionary bioinspired materials for optoelectronic functionalities. Melanin is a natural pigment distributed in vivo, and provides protection from the sun rays, exhibiting a strong wide-band UV–visible absorption. In the present study, we investigated the optical properties of natural melanin at different pH concentrations within the framework of experimental techniques, namely, UV–visible absorption, Fourier transform infrared spectroscopy (FTIR), and fluorescence spectroscopies. The results indicate that the optical absorption and fluorescence of natural melanin are enhanced within the near-UV and visible regimes with an increase in the solution concentration, are dependent on the pH level, and can impact the emergence of a broad band of visible absorption. The variations in the optical absorption spectra of natural melanin solutions at various pH levels will demonstrate novel rational strategies for controlling their optical properties for potential optoelectronic applications.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Comparison of total emitted solar-induced chlorophyll fluorescence (SIF) and top-of-canopy (TOC) SIF in estimating photosynthesis

We report many studies have shown that solar-induced fluorescence (SIF) has a good potential to predict gross primary production (GPP) of vegetation. What we measured by remote sensing or near-surface platforms is top-of-canopy (TOC) SIF (SIF toc ), which is not necessarily equal or proportional to total emitted SIF (SIF tot ) from the entire canopy due to the (re)absorption and scattering effects. However, photosynthesis, the process that plants use to fix carbon from the atmosphere, occurs at the entire vertical canopy. Here, by using the recollision theory, we calculated SIF tot at 760 nm from the measured SIF toc , hyperspectral reflectance (R), canopy interception (i) and leaf albedo (ω l ). Among them, both SIF toc and R can be obtained from concurrent TOC spectral measurements; i and ω l in the near-infrared region can be estimated from the open access datasets with a good accuracy. Our result confirms that the measured SIF toc only accounts for a small fraction of SIF tot : the above-the-canopy sensor can only “see” on average 22.9% of SIF tot at Harvard Forest. SIF tot has the following advantages over SIF toc in estimating GPP: (1) SIF tot improves the diurnal estimate of canopy GPP, especially capable to capture the midday depression of photosynthesis which may cause the large discrepancies between SIF toc and GPP on a diurnal basis, (2) SIF tot produces a stronger correlation with GPP from plants with complex canopy structure or under sky conditions with more diffuse irradiance, and (3) the SIF tot -GPP relationship shows a stronger resilience to environmental stresses. The fluorescence escape ratio (f esc ), the ratio between SIF toc multiplied by π and SIF tot , is mostly determined by the sun-canopy-sensor geometry and leaf inclination distribution. The effect of LAI and the leaf chlorophyll concentration on f esc is marginal at the 760 nm wavelength. Our results suggest that converting SIF toc into SIF tot provides a better tool to understand and estimate GPP.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2012

High energy resolution five-crystal spectrometer for high quality fluorescence and absorption measurements on an x-ray absorption spectroscopy beamline

Fluorescence detection is classically achieved with a solid state detector (SSD) on x-ray absorption spectroscopy (XAS) beamlines. This kind of detection however presents some limitations related to the limited energy resolution and saturation. Crystal analyzer spectrometers (CAS) based on a Johann-type geometry have been developed to overcome these limitations. We have tested and installed such a system on the BM30B/CRG-FAME XAS beamline at the ESRF dedicated to the structural investigation of very dilute systems in environmental, material and biological sciences. The spectrometer has been designed to be a mobile device for easy integration in multi-purpose hard x-ray synchrotron beamlines or even with a laboratory x-ray source. The CAS allows to collect x-ray photons from a large solid angle with five spherically bent crystals. It will cover a large energy range allowing to probe fluorescence lines characteristic of all the elements from Ca (Z = 20) to U (Z = 92). It provides an energy resolution of 1-2 eV. XAS spectroscopy is the main application of this device even if other spectroscopic techniques (RIXS, XES, XRS, etc.) can be also achieved with it. The performances of the CAS are illustrated by two experiments that are difficult or impossible to perform with SSD and the complementarity of the CAS vs SSD detectors is discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2013

Combined synchrotron X-ray tomography and X-ray powder diffraction using a fluorescing metal foil

This study realizes the concept of simultaneous micro-X-ray computed tomography and X-ray powder diffraction using a synchrotron beamline. A thin zinc metal foil was placed in the primary, monochromatic synchrotron beam to generate a divergent wave to propagate through the samples of interest onto a CCD detector for tomographic imaging, thus removing the need for large beam illumination and high spatial resolution detection. Both low density materials (kapton tubing and a piece of plant) and higher density materials (Egyptian faience) were investigated, and elemental contrast was explored for the example of Cu and Ni meshes. The viability of parallel powder diffraction using the direct beam transmitted through the foil was demonstrated. The outcomes of this study enable further development of the technique towards in situ tomography/diffraction studies combining micrometer and crystallographic length scales, and towards elemental contrast imaging and reconstruction methods using well defined fluorescence outputs from combinations of known fluorescence targets (elements).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2013

Measurement of XeI and XeII velocity in the near exit plane of a low-power Hall effect thruster by light induced fluorescence spectroscopy

Near exit plane non-resonant light induced fluorescence spectroscopy is performed in a Hall effect low-power Xenon thruster at discharge voltage of 250 V and anode flow rate of 0.7 mg/s. Measurements of the axial and radial velocity components are performed, exciting the 6s{sup 2}[3/2]{sub 2}{sup o}{yields}6p{sup 2}[3/2]{sub 2} transition at 823.16 nm in XeI and the 5d[4]{sub 7/2}{yields}6p[3]{sub 5/2}{sup o} transition at 834.724 nm in XeII. No significant deviation from the thermal velocity is observed for XeI. Two most probable ion velocities are registered at a given position with respect to the thruster axis, which are mainly attributed to different areas of creation of ions inside the acceleration channel. The spatial resolution of the set-up is limited by the laser beam size (radius of the order of 0.5 mm) and the fluorescence collection optics, which have a view spot diameter of 8 mm.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2014

Fluorescence modulation in single CdSe quantum dots by moderate applied electric fields

Single molecule time-resolved fluorescence spectroscopy of CdSe/ZnS core-shell quantum dots (QDs) under the influence of moderate applied electric fields reveals distributed emission from states which are neither fully on nor off and pronounced changes in the excited state decay. The data suggest that a 54 kV/cm applied electric field causes small perturbations to the QD surface charge distribution, effectively increasing the surface trapping probability and resulting in the appearance of gray states. We present simultaneous blinking and fluorescence decay results for two sets of QDs, with and without an applied electric field. Further kinetic modeling analysis suggests that a single trapped charged cannot be responsible for a blinking off event.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Laboratory-based micro-X-ray fluorescence setup using a von Hamos crystal spectrometer and a focused beam X-ray tube

The high-resolution von Hamos bent crystal spectrometer of the University of Fribourg was upgraded with a focused X-ray beam source with the aim of performing micro-sized X-ray fluorescence (XRF) measurements in the laboratory. The focused X-ray beam source integrates a collimating optics mounted on a low-power micro-spot X-ray tube and a focusing polycapillary half-lens placed in front of the sample. The performances of the setup were probed in terms of spatial and energy resolution. In particular, the fluorescence intensity and energy resolution of the von Hamos spectrometer equipped with the novel micro-focused X-ray source and a standard high-power water-cooled X-ray tube were compared. The XRF analysis capability of the new setup was assessed by measuring the dopant distribution within the core of Er-doped SiO{sub 2} optical fibers.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Optical and structural properties of plasma-treated Cordyceps bassiana spores as studied by circular dichroism, absorption, and fluorescence spectroscopy

To understand the killing mechanism of fungal spores by plasma treatment, the optical, structural, and biological properties of the insect pathogenic fungus Cordyceps bassiana spores were studied. A nonthermal atmospheric-pressure plasma jet (APPJ) was used to treat the spores in aqueous solution. Optical emission spectra of the APPJ acquired in air indicated emission peaks corresponding to hydroxyl radicals and atomic oxygen. When the APPJ entered the aqueous solution, additional reactive species were derived from the interaction of plasma radicals with the aqueous solution. Fluorescence and absorption spectroscopy confirmed the generation of hydroxyl radicals and hydrogen peroxide in the plasma-activated water (PAW). Spore counting showed that plasma treatment significantly reduced spore viability. Absorption spectroscopy, circular dichroism (CD) spectroscopy, and agarose gel electrophoresis of the DNA extracted from plasma-treated spores showed a reduction in spore DNA content. The magnitude of the dip in the CD spectrum was lower in the plasma-treated spores than in the control, indicating that plasma treatment causes structural modifications and/or damage to cellular components. Tryptophan fluorescence intensity was lower in the plasma-treated spores than in the control, suggesting that plasma treatment modified cell wall proteins. Changes in spore viability and DNA content were attributed to structural modification of the cell wall by reactive species coming from the APPJ and the PAW. Our results provided evidence that the plasma radicals and the derived reactive species play critical roles in fungal spore inactivation.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2015

Vibronic coupling in molecular crystals: A Franck-Condon Herzberg-Teller model of H-aggregate fluorescence based on quantum chemical cluster calculations

Here, we present a general approach to treating vibronic coupling in molecular crystals based on atomistic simulations of large clusters. Such clusters comprise model aggregates treated at the quantum chemical level embedded within a realistic environment treated at the molecular mechanics level. As we calculate ground and excited state equilibrium geometries and vibrational modes of model aggregates, our approach is able to capture effects arising from coupling to intermolecular degrees of freedom, absent from existing models relying on geometries and normal modes of single molecules. Using the geometries and vibrational modes of clusters, we are able to simulate the fluorescence spectra of aggregates for which the lowest excited state bears negligible oscillator strength (as is the case, e.g., ideal H-aggregates) by including both Franck-Condon (FC) and Herzberg-Teller (HT) vibronic transitions. The latter terms allow the adiabatic excited state of the cluster to couple with vibrations in a perturbative fashion via derivatives of the transition dipole moment along nuclear coordinates. While vibronic coupling simulations employing FC and HT terms are well established for single-molecules, to our knowledge this is the first time they are applied to molecular aggregates. Here, we apply this approach to the simulation of the low-temperature fluorescence spectrum of para-distyrylbenzene single-crystal H-aggregates and draw comparisons with coarse-grained Frenkel-Holstein approaches previously extensively applied to such systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2015

Optical-optical double resonance, laser induced fluorescence, and revision of the signs of the spin-spin constants of the boron carbide (BC) free radical

The cold boron carbide free radical (BC X {sup 4}Σ{sup −}) has been produced in a pulsed discharge free jet expansion using a precursor mixture of trimethylborane in high pressure argon. High resolution laser induced fluorescence spectra have been obtained for the B {sup 4}Σ{sup −}–X {sup 4}Σ{sup −} and E {sup 4}Π–X {sup 4}Σ{sup −} band systems of both {sup 11}BC and {sup 10}BC. An optical-optical double resonance (OODR) scheme was implemented to study the finer details of both band systems. This involved pumping a single rotational level of the B state with one laser and then recording the various allowed transitions from the intermediate B state to the final E state with a second laser by monitoring the subsequent E–X ultraviolet fluorescence. In this fashion, we were able to prove unambiguously that, contrary to previous studies, the spin-spin constant λ is negative in the ground state and positive in the B {sup 4}Σ{sup −} excited state. It has been shown that λ″ < 0 is in fact expected based on a semiempirical second order perturbation theory calculation of the magnitude of the spin-spin constant. The OODR spectra have also been used to validate our assignments of the complex and badly overlapped E {sup 4}Π–X {sup 4}Σ{sup −} 0-0 and 1-0 bands of {sup 11}BC. The E–X 0-0 band of {sup 10}BC was found to be severely perturbed. The ground state main electron configuration is …3σ{sup 2}4σ{sup 2}5σ{sup 1}1π{sup 2}2π{sup 0} and the derived bond lengths show that there is a 0.03 Å contraction in the B state, due to the promotion of an electron from the 4σ antibonding orbital to the 5σ bonding orbital. In contrast, the bond length elongates by 0.15 Å in the E state, a result of promoting an electron from the 5σ bonding orbital to the 2π antibonding orbitals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Laser-induced fluorescence of filament-produced plasmas

Self-guided ultrafast laser filaments are a promising method for laser beam delivery and plasma generation for standoff and remote detection of elements and isotopes via filament-induced breakdown spectroscopy (FIBS). Yet, there are several challenges associated with the practical application of FIBS, including delivery of sufficient laser energy at the target for generating plasma with a copious amount of emission signals for obtaining a high signal-to-noise ratio. Here, in this study, we use laser-induced fluorescence (LIF) to boost the emission signal and reduce self-reversal in the spectral profiles. Ultrafast laser filaments were used to produce plasmas from an Al 6061 alloy target at various standoff distances from 1 to 10 m. For LIF emission enhancement, a narrow linewidth continuous-wave laser was used in resonance with a 394.40 nm Al I resonant transition, and the emission signal was monitored from the directly coupled transition at 396.15 nm. Emission signal features of Al I are significantly enhanced by resonant excitation. In addition, LIF of filament ablation plumes reduces the self-reversal features seen in the thermally excited spectral profiles. Time-resolved two-dimensional fluorescence spectroscopy was performed for evaluating the optical saturation effects, which are found to be non-negligible due to high Al atomic densities in the filament-produced plasmas.

47 OTHER INSTRUMENTATION↗
DOE OSTI2019

Fluorescence and lasing in an electric-field-induced periodic structure of a cholesteric liquid crystal

Fluorescence and lasing in a structure with an electric-field-induced spatially periodic director modulation in the plane of a planar-oriented layer of a cholesteric liquid crystal (CLC) is experimentally investigated. The thickness of the CLC layer is chosen close to the natural pitch of the cholesteric helix, which corresponds to the second Grandjean zone. The electric-field-induced periodic field of the CLC director leads to spatial modulation of the refractive index and the appearance of optical properties typical of 1D photonic crystals, when light propagating in the plane of the CLC layer experiences Bragg reflection. In polarised light, the induced spatial modulation of the refractive index manifests itself in the form of banded domains oriented in the plane of the CLC layer perpendicular to the original (unperturbed electric field) direction of the director in the centre of the layer. For the electric field strengths that correspond to fundamentally different distributions of the field of a CLC director, the fluorescence spectra of the DCM laser dye are studied both for different geometries (including the waveguide regime) and for different levels of optical pumping. In the range of electrical voltages corresponding to the induction of a spatially periodic photonic structure, multimode lasing in the waveguide regime is detected. It is shown that the mode composition of lasing depends on the electric field, which affects the properties of the distributed feedback. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2017

Determination of copper nanoparticle size distributions with total reflection X-ray fluorescence spectroscopy

Total reflection X-ray fluorescence (TXRF) analysis is extensively used by the semiconductor industry for measuring trace metal contamination on silicon surfaces. In addition to determining the quantity of impurities on a surface, TXRF can reveal information about the vertical distribution of contaminants by measuring the fluorescence signal as a function of the angle of incidence. In this study, two samples were intentionally contaminated with copper in non-deoxygenated and deoxygenated ultrapure water (UPW) resulting in impurity profiles that were either atomically dispersed in a thin film or particle-like, respectively. The concentration profile of the samples immersed into deoxygenated UPW was calculated using a theoretical concentration profile representative of particles, yielding a mean particle height of 16.1 nm. However, the resulting theoretical profile suggested that a distribution of particle heights exists on the surface. The fit of the angular distribution data was further refined by minimizing the residual error of a least-squares fit employing a model with a Gaussian distribution of particle heights about the mean height. The presence of a height distribution was also confirmed with atomic force microscopy measurements.

36 MATERIALS SCIENCE↗