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DOE OSTI2020

MARCUS Ice Nucleating Particle Measurements (revised 7/2020)

These data list ice nucleating particle (INP) number concentrations active in the immersion freezing mode. Aerosol filters were collected during 4 voyages of the Aurora Australis vessel from 02 November 2017 to 22 March 2018, as part of the Measurements of Aerosols, Radiation and Clouds over the Southern Ocean (MARCUS) study. These voyages transected the Southern Ocean from Hobart, Tasmania to four Australian Antarctic Division stations, including three in Antarctica. Collections were made over alternating periods of 24 and 48 hours using open-faced polycarbonate filters that were approximately 18 m MSL, sited near the AOS trailer and other AMF measurements. The volume of air filtered ranged from 19000 to 38000 standard liters per filter sample. Filters were stored and returned frozen to Colorado State University (CSU), where immersion freezing measurements over a range from 0 to -28 degC were made using the CSU Ice Spectrometer (IS). Collected particles from each filter were resuspended in filtered, deionized water, and then dispensed into the IS and cooled to obtain cumulative INP temperature spectra. Aliquots of suspensions from selected samples were also heat treated (95 degC for 20 min) to denature and deactivate biological INPs, and digested in 10% H2O2 at 95 degC under UV-B for 20 min to remove all organic carbon INPs, prior to measurement using the IS.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1973

The reactions of HO2 with CO and NO and the reaction of O(1D) with H2O

HO2 radicals were generated by the photolysis of N2O at 2139 A in the presence of excess H2O or H2 and smaller amounts of CO and O2. The O(1D) atoms produced from the photolysis of N2O to give HO radicals or H2 to give HO + H. With H2O two HO radicals are produced for each O(1D) removed low pressures (i.e. approximately 20 torr H2O), but the HO yield drops as the pressure is raised. This drop is attributed to the insertion reaction: O(1D) + H2O + M yields H2O2 +M. The HO radicals generated can react with either CO or H2 to produce H atoms which then add to O2 to produce HO2. Two reactions are given for the reactions of the HO radicals, in the absence of NO.

Simonaitis, R.↗

NASA NTRS1974

Diurnal variations of HOx and NOx in the stratosphere

The diurnal variations of odd hydrogen (OH, HO2, H2O2) and odd nitrogen compounds (NO, NO2, HNO3) are investigated by using a one-dimensional time-dependent model containing both chemistry and eddy transport. These variations are discussed in terms of relevant processes.-

Whitten, R. C.↗

NASA NTRS1975

TC-2 post Helios experiment data review

Data are presented from a systems postflight analysis of the Centaur Launch Vehicle and Helios. Also given is a comparison of data from preflight analyses. Topics examined are: (1) propellant behavior; (2) helium usage; (3) propellant tank pressurization; (4) propellant tank thermodynamics; (5) component heating; thermal control; and thermal protection system; (6) main engine system; (7) H2O2 consumption; (8) boost pump post-meco performance; and (9) an overview of other systems.

Source record↗

NASA NTRS1975

Stratospheric distributions of odd nitrogen and odd hydrogen in a two-dimensional model

A two-dimensional pole-to-pole chemical model of the stratosphere is developed which extends from 8 to 38 km in altitude. Atmospheric motions are simulated by mean vertical and meridional winds and eddy diffusion coefficients. Seasonally averaged distributions of important odd nitrogen (NO, NO2, and HNO3) and odd hydrogen (H, OH, HO2, H2O2) compounds are computed. Photodissociation of N2O leads to production of odd nitrogen in the stratosphere, and the odd nitrogen is ultimately removed by downward transport into the troposphere and by rain-out (modeled by a rain-out lifetime of 30 days below 8-km altitude). Results are presented for a quasi-steady state in which seasonal cycles repeat themselves. These results show significant latitudinal as well as vertical variations in the predicted species which emphasize the need for at least two dimensions in accurate stratospheric modeling. Computed concentrations are compared with observations when they exist.

Prinn, R. G.↗

NASA NTRS1976

Effect of water vapor on the destruction of ozone in the stratosphere perturbed by ClX or NOx pollutants

Results are presented for a self-consistent one-dimensional coupled flow calculation for Ox, NOx, HOx, ClX, H2O, H2, CH4, H2O2, and N2O densities between 10 and 120 km. The results agree well with observations for the normal midlatitude atmosphere over this altitude range. ClX, NOx, and H2O are varied independently in the model considered. It is shown that the effect of depletion of ozone by ClX is to remove ozone preferentially above 30 km and to lower the altitude of maximum ozone density. This leads to enhanced solar heating of the lower stratosphere and tropopause and suggests the possibility of an increased flux of water into the stratosphere. Increasing water vapor in the stratosphere greatly enhances the rate of destruction of O3 by ClX and also causes an increase in the rate of destruction of O3 in the NOx-perturbed atmosphere.

Liu, S. C.↗

NASA NTRS1977

Photochemistry of the Martian atmosphere

A critical analysis is carried out for models which may be fine tuned to give agreement with observational constraints for O2, CO, and O3 in the Martian lower atmosphere and which are in accord also with upper atmospheric data for O and CO. The models have a number of features in common: dynamic mixing must be exceedingly rapid at heights above 90 km; if heterogeneous processes are not assumed to play a major role in the removal of atmospheric CO and O2, mixing must be rapid at heights between 30 and 40 km. The value implied for the diffusion coefficient in this region depends on the assumptions made regarding the rates for reaction of OH with HO2 to form H2O and the rate of reaction of HO2 with itself to form H2O2. If these reaction rates are taken to have values similar to those used in current models of the earth's stratosphere, the eddy diffusion coefficient at 40 km above the Martian surface should be about 5 by 10 to the seventh power sq cm/sec.

Kong, T. Y.↗

NASA NTRS1977

Ultraviolet absorption spectrum of hydrogen peroxide vapor

The ultraviolet absorption cross sections of hydrogen peroxide vapor have been determined over the wavelength range 210 to 350 nm at 296 K. At the longer wavelengths, the gas phase absorptivities are significantly larger than the corresponding values in condensed phase. The atmospheric H2O2 photodissociation rate for overhead sun at the earth's surface is estimated to be about 1.3 x 10 to the -5th/sec.

Molina, L. T.↗

NASA NTRS1978

Ultraviolet absorption cross sections of hydrogen peroxide

Absorption cross-sections of hydrogen peroxide vapor and of neutral aqueous solutions of hydrogen peroxide were measured in the wavelength range from 195 to 350 nm at 296 K. The spectrophotometric procedure is described, and the reported cross-sections are compared with values obtained by other researchers. Photodissociation coefficients of atmospheric H2O2 were calculated for direct absorption of unscattered solar radiation, and the vertical distributions of these coefficients are shown for various solar zenith angles.

Lin, C. L.↗

NASA NTRS1978

The Viking biological experiments on Mars

The three biological experiments on board the Viking Mars Landers are discussed. The gas exchange experiment provided periodic measurements of the composition and quantity of gases from Martian surface material, either in a humid or a wet nutrient sampling mode. The labeled release experiment demonstrated that adding an aqueous solution of dilute radioactive compounds to Martian material caused a rapid release of labeled gas. The results of the pyrolytic release experiment remain difficult to interpret. Data from the first two experiments suggest that oxidants (including H2O2 and iron oxide) rather than biota may account for all the observed reactions.

Klein, H. P.↗

NASA NTRS1979

The seasonal variation of ozone density in the Martian atmosphere

A one-dimensional, time-dependent model has been developed to investigate seasonal variations in ozone density in the Martian atmosphere. The model utilizes data for atmospheric temperature, pressure, and water vapor abundance observed by Viking. The results indicate that a high ozone density is not produced near the winter solstice but is in rather late winter, when the amount of water vapor is still small and the solar radiation can penetrate more deeply. A similar condition met in early winter does not necessarily produce a high ozone density because of the predicted higher HO2 density. Seasonal variations in ozone abundance are discussed in terms of the abundances of H2O and H2 and the seasonal variations in their reaction products H2O2 and HOx. The roles of transport, the effects of ozone loss to the surface, and the differences between northern and southern hemisphere ozone distributions are also discussed.

Shimazaki, T.↗

NASA NTRS1979

The evolution and variability of atmospheric ozone over geological time

The rise of atmospheric O3 as a function of the evolution of O2 has been investigated using a one-dimensional steady-state photochemical model based on the chemistry and photochemistry of Ox(O3, O, O(1D)), N2O, NOx(NO, NO2, HNO3), H2O, and HOx(H, OH, HO2, H2O2) including the effect of vertical eddy transport on the species distribution. The total O3 column density was found to maximize for an O2 level of 0.1 present atmospheric level (PAL) and exceeded the present total O3 column by about 40%. For that level of O2, surface and tropospheric O3 densities exceeded those of the present atmosphere by about an order of magnitude. Surface and tropospheric OH densities of the paleoatmosphere exceeded those of the present atmosphere by orders of magnitude. It was also found that in the O2-deficient paleoatmosphere, N2O (even at present atmospheric levels) produces much less NOx than it does in the present atmosphere.

Levine, J. S.↗

NASA NTRS1980

An experiment concept to measure stratospheric trace constituents by laser heterodyne spectroscopy

Laser heterodyne spectroscopy (LHS) techniques were used to measure radical gases from Spacelab. Major emphasis was placed on the measurement of ClO, ClOnO2, HO2, H2O2, N2O5, and HOCl in solar occultation with vertical resolution less than or equal to 2-km and vertical range from 1O to 70-km. Sensitivity analyses were performed on ClO and O3 to determine design criteria for the LHS instrument. Results indicate that O3 and ClO vertical profiles can be measured with an accuracy more than or equal to 95% and more than or equal to 80%, respectively, over the total profile.

Allario, F.↗

NASA NTRS1980

Sensitivity studies and laboratory measurements for the laser heterodyne spectrometer experiment

Several experiments involving spectral scanning interferometers and gas filter correlation radiometers (ref. 2) using limb scanning solar occultation techniques under development for measurements of stratospheric trace gases from Spacelab and satellite platforms are described. An experiment to measure stratospheric trace constituents by Laser Heterodyne Spectroscopy, a summary of sensitivity analyses, and supporting laboratory measurements are presented for O3, ClO, and H2O2 in which the instrument transfer function is modeled using a detailed optical receiver design.

Allario, F.↗

NASA NTRS1979

Heterogeneous atmospheric reactions - Sulfuric acid aerosols as tropospheric sinks

The reaction probabilities of various atmospheric species incident on a bulk sulfuric acid surface are measured in order to determine the role of sulfuric acid aerosols as pollutant sinks. Reaction products and unreacted starting materials leaving a Knudsen cell flow reactor after collision at 300 K with a H2SO4 surface or a soot surface were detected by mass spectrometry. Significant collision reaction probabilities are observed on a H2SO4 surface for H2O2, HNO3, HO2NO2, ClONO2, N2O5, H2O and NH3, and on soot for NH3. Estimates of the contribution of heterogeneous reactions to pollutant removal under atmospheric conditions indicate that while aerosol removal in the stratosphere is insignificant (loss rate constants approximately 10 to the -10th/sec), heterogeneous reactions may be the dominant loss process for several tropospheric species (loss rate constant approximately 10 to the -5th/sec, comparable to photolysis rate constants).

Baldwin, A. C.↗

NASA NTRS1979

Airborne laser induced fluorescence system for measuring OH and other trace gases in the parts-per-quadrillion to parts-per-trillion range

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.

Davis, D. D.↗

NASA NTRS1980

An experiment concept to measure stratospheric trace constituents by Laser Heterodyne Spectroscopy

The concept and techniques of a Laser Heterodyne Spectrometer experiment for measuring the vertical profiles of several stratospheric trace gases are discussed. The goal of the experiment is to develop a laser heterodyne receiver capable of measuring 2-4 gases simultaneously from Spacelab and, ultimately, from free-flying platforms. Sensitivity analyses are currently being performed for tenuous molecules such as ClO, ClONO2, NOCl, HO2, H2O2, and N2O5, although the capability exists for measuring more abundant gases, such as O3, HNO3, N2O, NO2, and CH4. Results indicate that O3 and ClO vertical profiles can be measured with an accuracy equal to or better than 95% and 80%, respectively, over the total profile. Laboratory measurements of the performance characteristics of the local oscillator and heterodyne detector are discussed with reference to 'excess-noise' and Doppler-shift effects.

Allario, F.↗

NASA NTRS1981

Measurement of HO2 and other trace gases in the stratosphere using a high resolution far infrared spectrometer at 28 Km

A progress report and data analyses from the December 1980 flight are presented. The following areas are covered: (1) computer analysis of the flight spectra to obtain phase corrected, normalized sums of spectra for retrieval of atmospheric profiles; (2) study of atmospheric HF, HCl, and H2O; (3) stratospheric H2O2 and HOCl; (4) laboratory spectroscopy of HOCl; and (5) design study of a new balloon gondola. The majority of the flight data were taken in the low background mode, i.e., one input to the spectrometer looking at the sky and the other looking at a LN2 temperature blackbody. An analysis of HF stratospheric measurements was undertaken in conjunction with the HF analysis. High quality spectra showing the HOCl q-branches under optically thin conditions were also obtained.

Traub, W. A.↗