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The fluorescence intensity of the H2 Lyman bands excited by the argon 1066 A line is found to be a linear function of the H2 pressure. The fluorescence from naturally occurring HD is linearly dependent on the HD partial pressure. The experiments described show that these fluorescence intensities can be used to measure the H2 and HD densities below 10 trillion molecules per cu cm.
The fluorescence of H2 in the Lyman band system, excited by solar extreme ultraviolet radiation, provides a means for the optical detection of H2 in the upper atmosphere. In particular, the Ly beta line of hydrogen is nearly degenerate with the (6,0) P1 transition, and absorption in this line produces fluorescence in the v-prime = 6 progression, principally at 1265, 1366, 1462 and 1608 A. Absorption by O2 rapidly attenuates the Ly beta from an overhead sun below 100 km and also significantly attenuates the fluorescent radiation. Far-ultraviolet dayglow spectra from 1130 to 1510 A obtained from an Aerobee rocket experiment on 11 December 1972 give an upper limit for any H2 emission which is a factor of 5 higher than expected according to recent hydrogen models.
Measurements of vacuum ultraviolet fluorescence from the photodissociation of CO2 by photons from a N IV line emission source at a wavelength of 923 A have revealed a second CO band system in addition to the expected emission bands. Spectra with time resolution were obtained and the fluorescence lifetime and the dependence of fluorescence intensity on CO2 pressure were measured. An analysis of this data has permitted the second band system to be identified as originating from CO(d-3 Delta sub i to X-1 Sigma +) transitions.
A lidar system is developed that uses four selected excitation wavelengths to induce chlorophyll 'a' fluorescence which is indicative of both the concentration and diversity of phytoplankton. The operating principles of the system and the results of measurements of phytoplankton fluorescence in a controlled laboratory environment are presented. A comparative study of results from lidar fluorosensor laboratory tank tests using representative species of phytoplankton in single and multispecies cultures from each of four color groups reveals that (1) there is good correlation between the fluorescence of chlorophyll 'a' remotely simulated and detected by the lidar system and in-situ measurements using four similar excitation wavelengths in a flow-through fluorometer; (2) good correlation exists between the total chlorophyll 'a' calculated from lidar-fluorosensor data and measurements obtained by the Strickland-Parsons method; and (3) the lidar fluorosensor can provide an index of population diversity.
The radiative transfer equation is modified to include the effect of fluorescent substances and solved in the quasi-single scattering approximation for a homogeneous ocean containing fluorescent particles with wavelength independent quantum efficiency and a Gaussian shaped emission line. The results are applied to the in vivo fluorescence of chlorophyll a (in phytoplankton) in the ocean to determine if the observed quantum efficiencies are large enough to explain the enhancement of the ocean's diffuse reflectance near 685 nm in chlorophyll rich waters without resorting to anomalous dispersion. The computations indicate that the required efficiencies are sufficiently low to account completely for the enhanced reflectance. The validity of the theory is further demonstrated by deriving values for the upwelling irradiance attenuation coefficient at 685 nm which are in close agreement with the observations.
Potential curves for the ground state and the first excited state of NaAr were determined. The van der Waals molecule NaAr was prepared by supersonic free jet expansion of a mixture of sodium, argon, and helium. The electronic transition from the ground state to the first excited state A2pi was excited by a tunable dye laser and the resulting fluorescence was studied. The dispersed fluorescence spectra show discrete and diffuse features, corresponding to transitions from excited vibrational levels of the A state to bound and unbound levels of the x state. The characteristic reflection structure in the bound-free spectra permits an unambiguous assignment of the vibrational numbering in the A state, and this assignment together with previously measured spectroscopic constants are used to calculate the potential curve of the A state. The discrete structure in the fluorescence spectra is used to determine the potential curve of the x state in the well region, and the repulsive part of the X curve is then deduced through trial-and-error simulation of the bound-free spectra.
Described in detail is a laser induced fluorescence system which has been successfully interfaced with two aircraft sampling platforms (i.e., Sabreliner jet and an L-188C Electra). This system, which has been under development for four years, presently consists of the following major components: (1) a Nd-Yag laser driven oscillator-amplifier dye laser; (2) a sampling manifold with associated fluorescence detection optics; (3) an OH calibration chamber; (4) a laser beam steering assembly; and (5) sampling electronics and data processing hardware. During the last three years, this system has been flown some 50,000 air miles making tropospheric OH radical measurements over the latitude range of 70 N to 57 S. OH concentrations measured during these flights have ranged from 30 parts-per-quadrillion (3.7 x 10 to the 5th molecules/sq cm) at altitudes of 6 km to 0.8 parts-per-trillion (2.0 x 10 to the 7th molecules/sq cm) at 0.5 km. Computations have been completed which indicate that the existing aircraft system with modest modifications should also be capable of detecting natural tropospheric levels of NO, SO2, CH2O, NO2, HNO2, NO3, H2O2 and CS2 by using both conventional laser-induced fluorescence methodology and multiphoton techniques.
Detailed fluorescence calculations for OH including the Swings effect were performed. These calculations were used to reproduce the high resolution spectra of Comets Seargent and Bradfield taken with IUE. The calculations also provide the OH fluorescence efficiencies (g factors), as a function of heliocentric radial velocity, which are needed to derive OH abundances from measured fluxes. A close examination of the spectra shows no sign of the corresponding emission bands of OD allowing upper limits to be placed on the ratio N(OD)/N(OH). Preliminary attempts to reproduce the CO+ band structure by fluorescence are discussed.
A new method for the in situ detection of nonfluorescing molecular species is proposed: photofragmentation-laser induced fluorescence (PF-LIF). In this approach, the species to be detected is first laser photolyzed at a wavelength lambda (1), producing one or more vibrationally excited photofragments. Before vibrational relaxation occurs, one of these photofragments is pumped into a bonding excited state by a second laser pulse centered at wavelength lambda (2). Fluorescence is sampled at a wavelength lambda (3), where lambda (3) is less then lambda (2) and lambda (1). This pumping configuration thus permits massive discrimination against Rayleigh and Raman scattering as well as white noise fluorescence from the laser wavelengths lambda (1) and lambda (2). The technique should be both highly sensitive and selective for numerous atmospheric trace gases. Specific sampling schemes for detecting NO2, NO3, and HNO2 are proposed. Various noise sources and chemical interferences are discussed. Specific calculations that estimate the sensitivity of the PF-LIF system for detecting NO2, NO3, and HNO2 are given.
The combined use of remote sensing and returned sample chemical data in lunar studies presumes a direct link between the two types of data. Laboratory experiments have demonstrated that within the precision of the lunar orbital X-ray fluorescence data there is a direct relationship between the fluorescence K-series X-radiation emitted from Mg, Al and Si in the surfaces of lunar soil samples and the concentrations of these elements in the bulk soil samples. This relationship encompasses both mare and terra soils. The degree of maturity is not an important variable for the existing orbital X-ray data. It is argued that these results are directly applicable to the lunar surface analyzed by the Apollo orbital X-ray fluorescence experiment.
An identification is made of a weak line in the high-resolution EUV solar spectrum, and the contribution of the Bowen fluorescence mechanism to line emission is considered. The line at 303.625 A is noted to coincide with the 2p 3d(3P2 0) - 2p2(3P1) transition of O III at 303.621 A, which could be excited by He II line excitation of the O III 2p2(3P2) - 2p 3d(3P2 0) transition at 303.799 A. Computations of the collisionally induced intensities of the 2p2(3P) - 2p3d(3P 0) multiplet are shown to result in values not observed in the solar spectrum, indicating that Bowen fluorescence, rather than collisional excitation, is the source of the line. The Bowen fluorescence mechanism is noted to have implications for the identification of other spectral lines, and for models of the solar corona.
A laser-induced fluorescence technique based on the pulsed two-photon excitation of NO is presented which is especially suited for the measurement of fluctuating temperatures in cold turbulent flows. The technique uses the fluorescence from the UV gamma bands of NO produced by two-photon excitation of NO (A 2 Sigma +, nu-prime = 0 - X 2 Pi, nu-double prime = 0) to obtain a rotational temperature. An analysis is presented of relevant aspects of the two-photon absorption process including microphysical processes, spectral intensities as a function of transition and laser spectral widths, line-shape integrals, the nonequilibrium response of the medium to a laser pulse, fluorescence energies, signal to noise ratio, and focusing effects. An analysis of absolute two-photon absorptivity measured in a nonflowing cell is then presented and used to predict signal to noise ratios greater than 50 for supersonic flows at temperatures below 300 K.
The process of H-Lyman-alpha fluorescence produced through photodissociation of CH4 and H2O provides an example for the usefulness of the detection of fluorescence of dissociation fragments as an aid in identifying some high lying Rydberg states. In the first experiment reported, an electron storage ring synchrotron radiation source was used. The fluorescence produced was detected with a solar blind photomultiplier and a Cs photocathode with a spectral sensitivity in the wavelength range from 1050 to 1950 A. In the second experiment considered, an intense atomic line source was employed.
Fluorescent emissions from nitric oxide appear imposed upon the Rayleigh backscattered spectrum of the earth's atmosphere between 250 and 300 nm in wavelength. Satellite instruments designed to monitor the global ozone distribution can routinely observe these signals although techniques for exploiting the data are not yet available. Application of a radiative transfer equation developed for an atmosphere including absorption by ozone, molecular scattering, and nitric oxide fluorescence shows the three most prominent NO emissions relative to the 250-300 nm backscattered sunlight to be the (1,4), (1,6), and (0,3) gamma bands. Analysis of the contribution function for each emission band indicates that the fluorescent signals can provide useful information on the magnitude and variability of nitric oxide between 40 and 140 km in altitude.
Airborne lidar oil spill experiments carried out to determine the practicability of the AOFSCE (absolute oil fluorescence spectral conversion efficiency) computational model are described. The results reveal that the model is suitable over a considerable range of oil film thicknesses provided the fluorescence efficiency of the oil does not approach the minimum detection sensitivity limitations of the lidar system. Separate airborne lidar experiments to demonstrate measurement of the water column Raman conversion efficiency are also conducted to ascertain the ultimate feasibility of converting such relative oil fluorescence to absolute values. Whereas the AOFSCE model is seen as highly promising, further airborne water column Raman conversion efficiency experiments with improved temporal or depth-resolved waveform calibration and software deconvolution techniques are thought necessary for a final determination of suitability.
The photoabsorption and fluorescence cross sections of CH4 were measured using synchrotron radiation at 1060-1420 A. The fluorescence starts to appear at 1330 A, and its cross section increases with decreasing photon wavelengths. The fluorescence cross section at 1060 A is 0.38 x 10 to the -18th sq cm, which is much smaller than the theoretical expectation. It is unlikely that the CH2 production from CH4 photodissociation will have a population inversion in the singlet system. A vibrational structure observed at 1060-1120 A is probably the 1t2-3p Rydberg transition of CH4.
Ultraviolet laser induced atomic fluorescence has been used to characterize supersonic jet aerodynamic levitation experiments. The levitated specimen was a 0.4 cm sapphire sphere that was separately heated at temperatures up to 2327 K by an infrared laser. The supersonic jet expansion and thermal gradients in the specimen wake were studied by measuring spatial variations in the concentration of atomic Hg added to the levitating argon gas stream. Further applications of atomic fluorescence in containerless experiments, such as ideal gas fluorescence thermometry and containerless process control are discussed.
The use of a laser-induced fluorescence technique for the sensitive measurement of the atmospheric hydroxyl radical is discussed. Results of laboratory studies of the fluorescence and other spectroscopic properties of OH which allow the calculation of OH concentrations from the returned signals for various altitudes, water vapor contents and temperatures are presented. The experimental setup used for airborne OH measurements is then described, with particular attention given to the use of a telescope for excitation and light collection in a coaxial configuration and the periodic tuning of the exciting radiation necessary to obtain an OH signal in the presence of strong solar and nonresonant fluorescence backgrounds. The best detection limit obtained to date with the system is noted to be about 700,000 OH/cu cm, and it is expected that, with planned improvements in detection and tuning schemes, limits in the neighborhood of 1,000,000 OH/cu cm will be achieved routinely.