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DOE OSTI2021

The “Brookhaven Brassie” and the Response to the Three Mile Island Accident

In the mid-1970s, American civil defense authorities became increasingly concerned with the potential threat of fission reactor accidents. Research from the Defense Civil Preparedness Agency began to be aimed not just at the ever-present threat of nuclear warfare, but also peacetime emergencies as part of a "dual use" philosophy. The Brookhaven National Laboratory received funding to create a prototype radioiodine air sampling system, with multiple publications detailing the creation of the air sampler itself and a special CD V-700 survey meter that accompanied it. In late March 1979, the system found its first operational employment at the reactor accident at Three Mile Island, Pennsylvania. Despite successful use and further study, the BNL Air Sampler was not widely fielded by the federal government. However, lessons learned from its employment and development may be applicable to contemporary radiological emergency response.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

NASA NTRS1985

Gas exchange and CO2 flux in the tropical Atlantic Ocean determined from Rn-222 and pCO2 measurements

The piston velocity for the tropical Atlantic Ocean has been determined from 29 radon profiles measured during the TTO Tropical Atlantic Study. By combining these data with the pCO2 data measured in the surface water and air samples, the net flux of CO2 across the sea-air interface has been calculated for the tropical Atlantic. The dependence of the piston velocity on wind speed is discussed, and possible causes for the high sea-to-air CO2 flux observed in the equatorial zone are examined.

Smethie, W. M., Jr.↗

DOE OSTI2025

A simple and practical wax-encapsulation method for air-sensitive XAS samples

To facilitate X-ray absorption spectroscopy (XAS) measurements of air-sensitive samples, we present a simple method in which materials are encased in common paraffin wax to protect them from air and moisture. We demonstrate the efficacy of this approach using a highly reducing, air- and moisture-sensitive uranium(III) complex, the tris(amide) U[N(SiMe 3 ) 2 ] 3 (1). When finely dispersed in a boron nitride matrix and subsequently encased in inert paraffin wax, samples of 1 remain stable with no visible or spectroscopic degradation after several days under ambient conditions. The viability of this method for XAS measurements was further evaluated across a series of uranium compounds, ranging from uranyl species to highly air- and moisture-sensitive molecular complexes, at the uranium L 3 -edge. Edge energy determinations were highly reproducible (±0.1 eV between replicates) and, where available, showed excellent agreement with literature values. In conclusion, this low-cost, effective, and versatile method offers a viable solution for XAS studies of air-sensitive compounds and materials.

36 MATERIALS SCIENCE↗

NASA NTRS2003

Toxicological Assessment of the International Space Station Atmosphere with Emphasis on Metox Canister Regeneration

Space-faring crews must have safe breathing air throughout their missions to ensure adequate performance and good health. Toxicological assessment of air quality depends on the standards that define acceptable air quality, measurements of pollutant levels during the flight, and reports from the crew on their in-flight perceptions of air quality. Air samples returned from ISS on flights 8A, UF2, 9A, and 11A were analyzed for trace pollutants. On average, the air during this period of operations was safe for human respiration. However, about 3 hours into the regeneration of 2 Metox canisters in the U.S. airlock on 20 February 2002 the crew reported an intolerable odor that caused them to stop the regeneration, take refuge in the Russian segment, and scrub air in the U.S. segment for 30 hours. Analytical data from grab samples taken during the incident showed that the pollutants released were characteristic of nominal air pollutants, but were present in much higher concentrations. The odors reported by the crew were due to relatively high concentrations of n-butanol, and possibly other pollutants in the mixture. Later data taken during regeneration of Metox canisters that had not been subject to long-term flows showed minimal effects on air quality. Long-term trending data suggest that a disruption in atmospheric mixing between the Service Module and the U.S. Laboratory has occurred and that formaldehyde concentrations are gradually increasing in the U.S. Laboratory. Trending data also show that the releases of octafluoropropane (OFP) have subsided.

James, John T.↗

NASA NTRS2001

An Assessment of the Ability of Potential Space-Borne Instruments to Resolve Spatial and Temporal Variability of Atmospheric Carbon Dioxide

Mounting concern regarding the possibility that increasing carbon dioxide concentrations will initiate climate change has stimulated interest in the feasibility of measuring CO2 mixing ratios from satellites. Currently, the most comprehensive set of atmospheric CO2 data is from the NOAA CMDL cooperative air sampling network, consisting of more than 40 sites where flasks of air are collected approximately weekly. Sporadic observations in the troposphere and stratosphere from airborne in situ and flask samplers are also available. Although the surface network is extensive, there is a dearth of data in the Southern Hemisphere and most of the stations were intentionally placed in remote areas, far from major sources. Sufficiently precise satellite observations with adequate spatial and temporal resolution would substantially increase our knowledge of the atmospheric CO2 distribution and would undoubtedly lead to improved understanding of the global carbon budget. We use a 3-D chemical transport model to investigate the ability of potential satellite instruments with a variety of orbits, horizontal resolution and vertical weighting functions to capture the variation in the modeled CO2 fields. The model is driven by analyzed winds from the Goddard Data Assimilation Office. Simulated CO2 fields are compared with existing surface and aircraft data, and the effects of the model convection scheme and representation of the planetary boundary layer are considered.

Andrews, Arlyn E.↗

NASA NTRS2003

Atmospheric Transport During the Transport and Chemical Evolution over the Pacific TRACE-P Experiment

Atmospheric transport over the Pacific Basin is described during NASA's Transport and Chemical Evolution Over the Pacific Experiment (TRACE-P) that was conducted between February - April 2001. The mission included extensive chemical sampling from two aircraft based primarily in Hong Kong and Yokota Air Base, Japan. Meteorological conditions during TRACE-P changed rapidly due to the seasonal winter/spring transition and the decay of prolonged ENSO cold phase (La Nina) conditions. To document these changes, TRACE-P was divided into two halves, and mean flow patterns during each half are presented and discussed. Important circulation features are the semi-permanent Siberian anticyclone and transient middle latitude cyclones that form near eastern Asia and then move eastward over the northern Pacific. Five-day backward trajectories from the various flight tracks show that air sampled by the aircraft had been transported from a variety of locations. Some parcels remained over the tropical western North Pacific during the entire period, while other important origins were Southeast Asia, Africa, and central Asia. Patterns of satellite-derived precipitation and lightning are described. TRACE-P occurs during a neutral to weak La Nina period of relatively cold sea surface temperatures in the tropical Pacific. Compared to climatology, the TRACE-P period exhibits deep convection located west of its typical position; however, tropospheric flow patterns do not exhibit a strong La Nina signal. Circulation patterns during TRACE-P are found to be generally similar to those during NASA's PEM WEST-B mission that occurred in the same region during February - March 1994.

Fuelberg, Henry E.↗

NASA NTRS2001

An Assessment of the Ability of Potential Spaceborne Instruments to Resolve Spatial and Temporal Variability of Atmospheric Carbon Dioxide

Andrews, Arlyn E.↗

DOE OSTI2012

Assessing Natural Isothiocyanate Air Emissions after Field Incorporation of Mustard Cover Crop

A regional air assessment was performed to characterize volatile natural isothiocyanate (NITC) compounds in air during soil incorporation of mustard cover crops in Washington State. Field air sampling and analytical methods were developed specific to three NITCs known to be present in air at appreciable concentrations during/after field incorporation. The maximum observed concentrations in air for the allyl, benzyl, and phenethyl isothiocyanates were respectively 188, 6.1, and 0.7 lg m-3 during mustard incorporation. Based on limited inhalation toxicity information, airborne NITC concentrations did not appear to pose an acute human inhalation exposure concern to field operators and bystanders.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2013

Solar Powered Radioactive Air Monitoring Stations

Environmental monitoring of ambient air for radioactive material is required as stipulated in the PNNL Site radioactive air license. Sampling ambient air at identified preferred locations could not be initially accomplished because utilities were not readily available. Therefore, solar powered environmental monitoring systems were considered as a possible option. PNNL purchased two 24-V DC solar powered environmental monitoring systems which consisted of solar panels, battery banks, and sampling units. During an approximate four month performance evaluation period, the solar stations operated satisfactorily at an on-site test location. They were subsequently relocated to their preferred locations in June 2012 where they continue to function adequately under the conditions found in Richland, Washington.

air sampling↗

DOE OSTI2020

High Throughput Argon-37 Field System

We report Pacific Northwest National Laboratory (PNNL) has developed a unique fieldable 37 Ar measurement system designed to measure 37 Ar activity concentrations from soil gas samples to detect above ground and underground nuclear explosions. The Argon-37 Field System is modular in design to accommodate both chemical processing and nuclear detection. The system can be packed into shipping crates and shipped to a location near where the sampling is taking place. The system can process six 2-m 3 whole-air samples in 24 hours and can measure the 37 Ar activity in each of the samples using six proportional counters. The proportional counters, designed and built at PNNL, are surrounded with both active and passive shielding to reduce background and can achieve a minimum detection concentration of 10 mBq/m 3 of 37 Ar in whole-air equivalent. The Argon-37 Field System has undergone extensive testing against rigorous requirements to assure the system meets the needs of the noble gas nuclear explosion monitoring community.

98 NUCLEAR DISARMAMENT, SAFEGUARDS, AND PHYSICAL P↗

NASA NTRS1986

Tropospheric HO determination by FAGE

In the detection of tropospheric HO by laser excited fluorescence, and alternative air-sampling method, named FAGE (Fluorescence Assay with Gas Expansion) was introduced. Here the air is expanded through a nozzle prior to excitation, in order to improve the ratio of the HO signal to the scattered, fluorescent, and photolytic backgrounds. The improvement comes from the differing pressure dependence of the intensities of these four terms, as well as the distinguishability of their temporal waveforms at low pressures when excited by a pulsed laser. HO has been excited by a YAG/dye laser. Other lasers and pumping paths may perform as well or better in this method. With FAGE, chemical modulation of the HO signal was achieved by hydrocarbon addition to the nozzle flow, converting photolytic HO from an interference to a background. Chemical calibration of the instrumental response to external HO was also achieved, by hydrocarbon decay, at HO concentrations within the ambient range.

Hard, T. M.↗

NASA NTRS1989

Carbon-14 in methane sources and in atmospheric methane - The contribution from fossil carbon

Measurements of carbon-14 in small samples of methane from major biogenic sources, from biomass burning, and in clean air samples from both the Northern and Southern hemispheres reveal that methane from ruminants contains contemporary carbon, whereas that from wetlands, peat bogs, rice fields, and tundra, is somewhat depleted in carbon-14. Atmospheric (C-14)H4 seems to have increased from 1986 to 1987, and levels at the end of 1987 were 123.3 + or - 0.8 percent modern carbon in the Northern Hemisphere and 120.0 + or - 0.7 percent modern carbon in the Southern Hemisphere.

Wahlen, M.↗

NASA NTRS1985

Measurements of CCl3F, CCl2F2, CCl4, N2O and SF6 in the Northern Hemisphere stratosphere

An overview of the Department of Energy's High Altitude Sampling Program and some recent trace gas measurement results are presented. Analysis of whole air samples, collected in pressurized bottles, provides information on stratospheric inventories and distributions for CCl3F, CCl2F2, CCl4, N2O and SF6 in the Northern Hemisphere. Based on a linear regression analysis of the data the estimated mean Northern Hemisphere stratospheric concentration of each gas increased as follows: CCl3F changed from 54 to 142 p1/1 (4/74-11/83); CCl2F2 changed from 133 to 268 p1/1 (4/76-11/83); SF6 changed from 160 to 480 f1/1 (4/74-11/83); CC1, changed from 58 to 91 p1/1 (4/75-11/83); N2O changed from 246 to 261 n1/1 (4/76-11/83). The calculated mean Northern Hemisphere stratospheric concentrations of N2O, CCl3F, CCl2F2, and CCl4 after 1980 show larger than expected fluctuations with time. Recent volcanic activity may be a partial cause for these fluctuations through induced changes in stratospheric dynamical processes.

Leifer, R.↗

NASA NTRS1996

Fungal colonization of fiberglass insulation in the air distribution system of a multi-story office building: VOC production and possible relationship to a sick building syndrome

Complaints characteristic of those for sick building syndrome prompted mycological investigations of a modern multi-story office building on the Gulf coast in the Southeastern United States (Houston-Galveston area). The air handling units and fiberglass duct liner of the heating, ventilating and air conditioning system of the building, without a history of catastrophic or chronic water damage, demonstrated extensive colonization with Penicillium spp and Cladosporium herbarum. Although dense fungal growth was observed on surfaces within the heating-cooling system, most air samples yielded fewer than 200 CFU m-3. Several volatile compounds found in the building air were released also from colonized fiberglass. Removal of colonized insulation from the floor receiving the majority of complaints of mouldy air and continuous operation of the units supplying this floor resulted in a reduction in the number of complaints.

NASA Program Environmental Health↗

DOE OSTI2024

Sulfuric Acid New Particle Formation Field Campaign Report

This campaign aimed to measure gaseous sulfuric acid concentrations at the surface level using a newly developed sulfuric acid dimethylamine-reactive condensation particle counter (SAD-RCPC). Sulfuric acid is a key nucleation precursor and is the likely driving compound for new particle formation at the Atmospheric Radiation Measurement (ARM) user facility’s Southern Great Plains (SGP) observatory. The SAD-RCPC will be deployed in the future at ARM SGP (AFC010010: "Vertically Resolved Nucleation Precursors at SGP") scheduled for 2024. The campaign was in conjunction with Eleanor Browne's campaign (AFC010075: Boundary-layer gradients in new particle formation) and took place from 05/7/23 to 5/21/23. The measured sulfuric acid concentrations by the SAD-RCPC will be compared to concentrations measured by Browne's chemical ionization mass spectrometer (CIMS). The SAD-RCPC consisted of a glass flow reactor coupled to a 1-nm diethylene glycol condensation particle counter (DEG CPC). Sampled air was mixed with a high concentration of dimethylamine vapor (~1 ppbv). Sulfuric acid within the sampled gas nucleated with dimethylamine to form detectable 1-nm particles. The measured particle concentration was converted to sulfuric acid concentration using nucleation reaction kinetics. The pulse height distribution of particles detected by the DEG CPC was observed using a multi-channel analyzer. Large pre-existing particles were separated from the freshly formed particles in the SAD-RCPC from the pulse height distribution (PHD). During the short campaign, seven new particle formation events were observed. The SAD-RCPC detected an increase in sulfuric acid concentration, but this also coincided with an increase in pre-existing <3 nm particle concentrations. In addition, Browne's CIMS detect sulfuric acid concentrations in the range of 10 5 -10 6 cm -3 .

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Measurement of Argon-37 Background Concentrations in the Atmosphere

Radioisotopes of noble gases, primarily xenon and argon, are important indicators of underground nuclear explosions. The Comprehensive Nuclear-Test-Ban Treaty (CTBT) includes monitoring capabilities to identify potential nuclear explosions conducted in violation of the CTBT. This monitoring currently focuses on measurement of the xenon isotopes 133 Xe, 135 Xe, 131 mXe and 133 mXe. However, it is predicted that within 100 days of an underground nuclear explosion (UNE) 37 Ar would be released to the atmosphere at higher concentrations than xenon isotopes (Haas et al. 2010). Therefore, inclusion of 37 Ar measurement capabilities at atmospheric International Monitoring System (IMS) stations could improve the capability to detect a nuclear explosion. At an IMS station, it could be difficult to determine what constitutes an elevated concentration as a result of an UNE without first understanding the expected range of background concentrations. This work describes our analysis of atmospheric samples for 37 Ar to evaluate the range of background concentrations. The range of 37 Ar concentrations measured in atmospheric air samples was relatively narrow ranging between less than 1 mBq/m 3 to greater than 2 mBq/m 3 . The average atmospheric concentration of all samples was 0.98 mBq/m 3 , with a standard deviation of 0.5 mBq/m 3 . This is consistent with previous published results. The results presented here demonstrate the capability to detect background concentrations of 37 Ar in atmospheric air.

61 RADIATION PROTECTION AND DOSIMETRY↗

DOE OSTI2025

Imprint of Anthropogenic Sources and Soil Removal on the Surface Concentration of H2 in the Contiguous US

Hydrogen (H2) is experiencing renewed interest throughout the world as a low carbon fuel alternative or complement to fossil fuels. Significant uncertainties remain regarding the environmental impact of increasing H2 usage, in part due to gaps in our understanding of the H2 atmospheric budget, including the H2 release from industrial activities and the H2 soil removal, the most important sink of H2. This study focuses on H2 dry air mole fractions measured by the NOAA Global Monitoring Laboratory in discrete ambient air samples collected every few days at sites located in the contiguous United States between 2010 and 2022. We take advantage of the long-term observations from this network to study the regional distribution of H2 sources using the potential source contribution function (PSCF). We find that H2 PSCF is consistent with a large anthropogenic source of atmospheric H2 from the incomplete combustion of fossil fuel. However, episodic air masses with high H2 dry air mole fractions (>700 ppb) recorded at some sampling locations in the Western and Southeastern US are not associated with elevated CO, suggesting significant noncombustion anthropogenic or geological sources of H2. Air masses depleted in H2 are recorded in rural or remote continental sites. Our analysis of observations from a tall tower in NE Colorado suggests that the degree of H2 depletion not only reflects differences in soil exposure but also the regional inhibition of the soil sink under arid conditions.

Paulot, Fabien↗

DOE OSTI2015

Short-lived species detection of nitrous acid by external-cavity quantum cascade laser based quartz-enhanced photoacoustic absorption spectroscopy

Spectroscopic detection of short-lived gaseous nitrous acid (HONO) at 1254.85 cm{sup −1} was realized by off-beam coupled quartz-enhanced photoacoustic spectroscopy (QEPAS) in conjunction with an external cavity quantum cascade lasers (EC-QCL). High sensitivity monitoring of HONO was performed within a very small gas-sample volume (of ∼40 mm{sup 3}) allowing a significant reduction (of about 4 orders of magnitude) of air sampling residence time which is highly desired for accurate quantification of chemically reactive short-lived species. Calibration of the developed QEPAS-based HONO sensor was carried out by means of lab-generated HONO samples whose concentrations were determined by direct absorption spectroscopy involving a ∼109.5 m multipass cell and a distributed feedback QCL. A minimum detection limit (MDL) of 66 ppbv (1 σ) HONO was achieved at 70 mbar using a laser output power of 50 mW and 1 s integration time, which corresponded to a normalized noise equivalent absorption coefficient of 3.6 × 10{sup −8 }cm{sup −1} W/Hz{sup 1/2}. This MDL was down to 7 ppbv at the optimal integration time of 150 s. The corresponding 1σ minimum detected absorption coefficient is ∼1.1 × 10{sup −7 }cm{sup −1} (MDL ∼ 3 ppbv) in 1 s and ∼1.1 × 10{sup −8 }cm{sup −1} (MDL ∼ 330 pptv) in 150 s, respectively, with 1 W laser power.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗