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DOE OSTI2023

SPRUCE Sphagnum Phytobiome Responses to Whole Ecosystem Warming and Elevated Atmospheric CO2 in July, 2017-2021

This dataset reports the carbon (C) and nitrogen (N) isotopic composition of Sphagnum moss tissue collected from the Spruce and Peatland Responses Under Changing Environments (SPRUCE) experimental site within the Marcell Experimental Forest in northern Minnesota, USA. Tissues were collected inside the SPRUCE experimental study plot, where air and peat warming are combined in whole-ecosystem warming treatments, from 2019-2021. Additionally, rates of nitrogen fixation and methane oxidation measured for Sphagnum from 2017, 2019, and 2021. Sphagnum tissue % water content was measured at all timepoints. This dataset was used to conduct analyses within Petro et al (2023). Sphagnum C and N concentrations and 13C and 15N isotopic natural abundance were determined for three replicate Sphagnum tissue samples collected from inside the SPRUCE enclosures in July 2019-2021. Elemental and isotope analyses were conducted at the University of Georgia – Center for Applied Isotope Studies (CAIS; https://cais.uga.edu/). Plant elemental analysis was performed by the micro-Dumas method, while isotopic natural abundance was measured by isotope ratio mass spectrometry. 13C natural abundance is expressed as the per mille (‰) deviation from the Pee Dee Belemnite standard (PDB) 13C:12C ratio (δ13C), while 15N natural abundance is expressed as the ‰ deviation from the N2 atmospheric 15N:14N ratio (δ15N). Rates of nitrogen fixation and methane oxidation were measured using serum bottle incubations performed with Sphagnum collected inside the SPRUCE enclosures in July 2017, 2019, and 2021. Rates were calculated according to the amount of 15N-N2 or 13C-CH4 (methane) incorporated into the Sphagnum tissue or incubation headspace over the 48-hour intion period. In 2017, incubations were performed in growth chambers set to the temperature of the experimental plots during Sphagnum sampling. In 2019 and 2021, the incubations were performed directly inside the experimental plots. The 13C and 15N isotopic natural abundance data and rate measurements presented in this dataset provide insight into the impacts of whole-ecosystem warming and elevated atmospheric carbon dioxide (CO2) on N and C cycling within the Sphagnum phytobiome. This dataset contains two data files in comma-separate values (*.csv) format. Additional metadata are provided: two data dictionaries and a file-level metadata file in comma-separate values (.csv) format and a user guide in PDF (*.pdf) format. Additional datasets on NH4-N availability, porewater concentrations of CH4 and CO2, and Sphagnum groundcover within the SPRUCE experimental plots are available. These are outlined in the Related Datasets section in the user guide.

delta 13 carbon↗

DOE OSTI2021

Fine Aerosol Acidity and Water during Summer in the Eastern North Atlantic

Aerosol pH governs many important atmospheric processes that occur in the marine boundary layer, including regulating halogen and sulfur chemistries, and nutrient fertilization of surface ocean waters. In this study, we investigated the acidity of PM1 over the eastern North Atlantic during the Aerosol and Cloud Experiments in Eastern North Atlantic (ACE-ENA) aircraft campaign. The ISORROPIA-II thermodynamic model was used to predict PM1 pH and water. We first investigated the sensitivities of PM1 pH and water predictions to gas-phase NH3 and HNO3 concentrations. Our sensitivity analysis indicated that even though NH3 and HNO3 were present at very low concentrations in the eastern North Atlantic during the campaign, PM1 pH calculations can still be sensitive to NH3 concentrations. Specifically, NH3 was needed to constrain the pH of populations of PM1 that had low mass concentrations of NH4+ and non-volatile cations (NVCs). We next assumed that gas-phase NH3 and HNO3 concentrations during the campaign were 0.15 and 0.09 µg m−3, respectively, based on previous measurements conducted in the eastern North Atlantic. Using the assumption that PM1 were internally mixed (i.e., bulk PM1), we determined that PM1 pH ranged from 0.3–8.6, with a mean pH of 5.0 ± 2.3. The pH depended on both Hair+ and Wi. Hair+ was controlled primarily by the NVCs/SO42− molar ratio, while Wi was controlled by the SO42− mass concentration and RH. Changes in pH with altitude were driven primarily by changes in SO42−. Since aerosols in marine atmospheres are rarely internally mixed, the scenario where non-sea salt species and sea-salt species were present in two separate aerosol modes in the PM1 (i.e., completely externally mixed) was also considered. Smaller pH values were predicted for the aerosol mode comprised only of non-sea salt species compared to the bulk PM1 (difference of around 1 unit on average). This was due to the exclusion of sea-salt species (especially hygroscopic alkaline NVCs) in this aerosol mode, which led to increases in Hair+ values and decreases in Wi values. This result demonstrated that assumptions of aerosol mixing states can impact aerosol pH predictions substantially, which will have important implications for evaluating the nature and magnitude of pH-dependent atmospheric processes that occur in the marine boundary layer.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Data from: Nitrification is a minor source of nitrous oxide (N2O) in an agricultural landscape and declines with increasing management intensity

The long-term contribution of nitrification to nitrous oxide (N2O) emissions from terrestrial ecosystems is poorly known and thus poorly constrained in biogeochemical models. Here, using Bayesian inference to couple 25 years of in situ N2O flux measurements with site-specific Michaelis-Menten kinetics of nitrification-derived N2O, we test the relative importance of nitrification-derived N2O across six cropped and unmanaged ecosystems along a management intensity gradient in the U.S. Midwest. We found that the maximum potential contribution from nitrification to in situ N2O fluxes was 13-17% in a conventionally fertilized annual cropping system, 27-42% in a low-input cover-cropped annual cropping system, and 52-63% in perennial systems including a late successional deciduous forest. Actual values are likely to be less than 10% of these values because of low N2O yields in cultured nitrifiers (typically 0.04 to 8% of NH3 oxidized) and competing sinks for available NH4+ in situ. Most nitrification-derived N2O was produced by ammonia oxidizing bacteria (AOB) rather than archaea (AOA), who appeared responsible for no more than 30% of nitrification-derived N2O production in all but one ecosystem. Although the proportion of nitrification-derived N2O production was lowest in annual cropping systems, these ecosystems nevertheless produced more nitrification-derived N2O (higher Vmax) than perennial and successional ecosystems. We conclude that nitrification is minor relative to other sources of N2O in all ecosystems examined.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Size resolved particle hygroscopcity for 30, 60, and 90 nm particles collected at the EPCAPE Mount Soledad site from 04/20/2023 to 06/15/2023

Contains both the growth factor probability density function (probability is out of 200) and the average growth factors calculated by the Gysel inversion. The instrument measured three different diameters 30 nm, 60nm and 90nm each diameter was selected for an hour. During that hour, five 12-minute scans were taken scanning growth factors from 0.5-3.0. RH was consistently kept at 85%. Calibrations of the instrument with NaCl were performed on 4/26/2023 from 11:20 to 14:20, on 5/16/2023 from 11:40 to 16:00, and on 5/30/2023 from 10:20 to 14:20. Calibrations with (NH4)2SO4 were performed on 5/8/2023 from 11:45 to 14:40, on 5/23/2023 from 11:20 to 3:00, and on 6/14/2023 from 13:00 to 16:00. Time is recorded in seconds since 1/1/1904.

30 nm particle hygroscopicity↗

DOE OSTI2025

Aerosol Thermodynamics (Aerosol Liquid Water Concentration and Aerosol pH) at S2 during CoURAGE

These data report aerosol liquid water content (ALWC) and aerosol pH for the S2 (Mt. Airy) site during CoURAGE for April - June 2025. The ISORROPIA-II aerosol thermodynamic equilibrium model was used to compute ALWC and pH. The model was run in forward mode, with solids formation disabled (metastable mode), according to Pye et al. (Atmospheric Chemistry and Physics, 2020). Information about the model can be found at https://www.epfl.ch/labs/lapi/models-and-software/isorropia/, and in Fountoukis and Nenes (Atmospheric Chemistry and Physics, 2007). Inputs to the model were: (1) measured Temperature and relative humidity, both from the DoE ARM “metwxt” data products at S2, (2) aerosol chemical composition from the ARM ACSM, and (3) gas-phase ammonia concentrations. For ISORROPIA-II, ambient RH values above 0.995 were input to the model as 0.995; therefore, caution should be exercised interpreting ALWC when RH was above 0.995. Aerosol composition or NH3(g) concentrations below the LOD were input into the model as 0.5*LOD. Model runs were only conducted for data points at 30-min resolution with all three inputs (meteorology, ACSM, and NH3). If any of the three model inputs were missing, aerosol thermodynamic outputs are flagged as -999. Similarly, aerosol thermodynamic outputs are flagged as -999 if measured NH3(g) and aerosol ammonium (NH4+) were simultaneously below the respective LODs. The ALWC includes liquid water from inorganic aerosol components, calculated directly by ISORROPIA-II, as well as liquid water from organics, estimated from the ACSM organics assuming a kappa value of 0.12 according to Guo et al. (Atmospheric Chemistry and Physics, 2015).

Aerosol Liquid Water Content↗

NASA NTRS1971

Specular reflectance of aqueous solutions.

Description of two laboratory instruments for measuring the specular reflectance of aqueous solutions. The instruments are an organic-dye-laser spectrophotometer for the 360- to 650-nm wavelength region and a reflectometer accessory for a Perkin-Elmer E-system spectrophotometer which will operate in the 0.2- to 20-micron wavelength region. The reflectometer accessory has been used to measure the relative infrared specular reflectance in limited spectral regions for aqueous solutions of NaCl, K2SO4, ZnSO4, (NH4)2SO4, and NH4H2PO4 with radiant flux incident at about 70 deg and polarized perpendicular to the plane of incidence. The laser spectrometer has been used to measure the absolute reflectance of aqueous solutions of NaCl in the wavelength region from 575 to 610 nm for light incident at angles of about 60, 65, and 70 deg and polarized parallel to the plane of incidence.

Querry, M. R.↗

NASA NTRS1973

Struvite and prebiotic phosphorylation.

Struvite rather than apatite or amorphous calcium phosphate is precipitated when phosphate is added to seawater containing more than 0.01M NH4+ ions. Struvite may have precipitated from evaporating seawater on the primitive earth, and may have been important for prebiotic phosphorylation.

Handschuh, G. J.↗

NASA NTRS1974

Cometary coma ions

For comets whose nuclei are composed of water ice conglomerates it is shown that the ion H3O(+) can predominate to distances of 5000 km in the subsolar direction. Beyond this distance H2O(+) is the most important ion. The crossover point is a sensitive function of the rate of evaporation from the nucleus. The presence of ammonia or metals such as sodium, in concentrations greater than 0.1% H2O, can lead to NH4(+) and Na(+) ions.

Aikin, A. C.↗

NASA NTRS1974

Cometary coma ions

Aikin, A. C.↗

NASA NTRS1976

Studies on the nature of plasma growth hormone

The paper presents further evidence for the existence of two discrete forms of growth hormone in human plasma, one which is detectable by both radioimmunoassay and bioassay and is immunoreactive, and the other, termed 'bioactive', which is detected by tibial bioassay but shows little reactivity with currently available antisera to pituitary growth hormone. The same division of immunoactive and bioactive growth hormone occurs in rats, though with less disparity. Tests on rats indicated that the bioactive hormone is preferentially released into jugular vein plasma and that plasma concentrations of the bioactive hormone can be enhanced by insulin administration. The bioactive hormone was detectable by tibial assays in Cohn fractions IV, IV-1, and IV-4, and could be concentrated about 40-fold by fractionation with (NaPO3)6 and (NH4)2SO4.

Ellis, S.↗

NASA NTRS1976

Crossed beam studies of ion-molecule reactions in methane and ammonia

A crossed-beam apparatus is used to measure the product ion velocity and angular distributions for the following ion-molecule reactions in the relative energy range from 2 to 9 eV: CH4(+) + NH3 yields NH4(+) + CH3; CH4(+) + NH3 yields CNH5(+) + H2; NH2(+) + CH4 yields CNH4(+) + H2 (or 2H); and CH3(+) + NH3 yields CNH4(+) + H2 (or 2H). These reactions are also studied by means of deuterium labeling as a further probe of the detailed reaction dynamics. Probability contour plots for the four reactions are constructed in Cartesian velocity space, and product peaks in the plots are discussed. Relative cross sections and Q values are computed for two of the reactions as well as for the corresponding deuterium-labelled reactions. The results show that the present ion-neutral condensation reactions are highly exothermic with a deep well for the internal complex, that little hydrogen scrambling occurs, and that the energy of the reactions is released mainly as internal energy, even to the extent of producing two hydrogen atoms in some cases rather than one hydrogen atom or molecule.

Smith, G. P. K.↗

NASA NTRS1977

Optical constants of ammonium sulfate in the infrared

The infrared spectral reflectance at near normal incidence has been measured for 3.2 M, 2.4 M, and 1.6 M solutions of ammonium sulfate, an aerosol abundant in the stratosphere and also present in the troposphere. Kramers-Kronig analysis was used to determine values of the refractive and absorption indices from the measured spectral reflectance. A synthetic spectrum of crystalline ammonium sulfate was obtained by extrapolation of the absorption index obtained for the solution to the absorber number densities of the NH4 and SO4 ions characteristic of the crystal.

Downing, H. D.↗

NASA NTRS1978

Rain scavenging of solid rocket exhaust clouds

An explicit model for cloud microphysics was developed for application to the problem of co-condensation/vaporization of HCl and H2O in the presence of Al2O3 particulate nuclei. Validity of the explicit model relative to the implicit model, which has been customarily applied to atmospheric cloud studies, was demonstrated by parallel computations of H2O condensation upon (NH4)2 SO4 nuclei. A mesoscale predictive model designed to account for the impact of wet processes on atmospheric dynamics is also under development. Input data specifying the equilibrium state of HC1 and H2O vapors in contact with aqueous HC1 solutions were found to be limited, particularly in respect to temperature range.

Dingle, A. N.↗

NASA NTRS1978

Infrared band intensities in ammonium hydroxide and ammonium salts

We have applied Kramers-Kronig analysis to reflection spectra to determine the optical constants of ammonium hydroxide and of aqueous solutions of ammonium chloride and bromide. From considerations of the absorption indices k(nu) we conclude that ammonium hydroxide consists of a solution of NH3 in water, in which NH3 molecules are hydrogen bonded to neighboring water molecules. The spectrum of ammonium hydroxide differs from the spectra of ammonium salts, in which bands characteristic of NH4(+) ions are prominent. The existence of ammonium hydroxide as an aerosol in planetary atmospheres is briefly discussed

Sethna, P. P.↗

NASA NTRS1978

Infrared band intensities of saturated hydrocarbons

Kramers-Kronig analysis is applied to measured values of spectral reflectance at near-normal incidence to determine the real and the imaginary parts of the complex index of refraction for methane, ethane, propane, n-butane, n-hexane, n-heptane, and n-decane in the liquid state. The results indicate that the strengths of the characteristic bands as measured by the integral of the imaginary part are roughly constant for all the liquid alkanes except for methane. The intensity of the CH valence vibration bands in the spectra of the alkanes except methane is directly proportional to the number of CH groups per unit volume. The relations for the intensity of the bands due to CH2 and CH3 deformations are examined. Characteristic band intensities of the type established for NH4(+) and SO4(2-) groups in solutions and crystals cannot be extended to the more closely coupled CH2 and CH3 groups in alkane molecules.

Pinkley, L. W.↗

NASA NTRS1979

Cosmic ray ionization of the Jovian atmosphere

An approximate form of the Boltzmann equation has been used to obtain local ionization rates due to the absorption of galactic cosmic rays in the Jovian atmosphere. It is shown that the muon flux component of the cosmic-ray-induced cascade may be especially important in ionizing the atmosphere at levels where the total number density exceeds 10 to the 19th per cu cm (well below the ionospheric layers produced by solar EUV). A model containing both positive and negative ion reactions has been employed to compute electron and ion number densities. Peak electron number densities of the order of 1000 per cu cm may be expected even at relatively low magnetic latitudes. The dominant positive ions are NH4(+) and CnHm(+) cluster ions, with n at least 2; it is suggested that the absorption of galactic cosmic-ray energy at such relatively high pressures in the Jovian atmosphere (M about 10 to the 18th to 10 to the 20th per cu cm) and the subsequent chemical reactions may be instrumental in the local formation of complex hydrocarbons.

Capone, L. A.↗

NASA NTRS1981

Advection fog formation in a polluted atmosphere

Large quantities of atmospheric aerosols with compositions SO4(2-), NO3(-) and NH4(+) have been detected in highly industrialized areas. The major portions of aerosol products are the results of energy-related fuel combustion. Both microphysical and macrophysical processes are considered in investigating the time-dependent evolution of the saturation spectra of condensation nuclei associated with both polluted and clean atmospheres during the time periods of advection fog formation. The results show that the condensation nuclei associated with a polluted atmosphere provide more favorable conditions than condensation nuclei associated with a clean atmosphere to produce dense advection fog, and that attaining a certain degree of supersaturation is not necessarily required for the formation of advection fog with condensation nuclei associated with a polluted atmosphere for monodisperse distribution.

Hung, R. J.↗

NASA NTRS1980

Fluid mechanics simulation of fog formation associated with polluted atmosphere produced by energy related fuel combustion

It is noted that large quantities of atmospheric aerosols with composition SO4(-2), NO3(-1), and NH4(+1) have been detected in highly industrialized areas. Most aerosol products come from energy-related fuel combustion. Fluid mechanics simulation of both microphysical and macrophysical processes is considered in studying the time dependent evolution of the saturation spectra of condensation nuclei associated with polluted and clean atmospheres during the time periods of advection fog formation. The results demonstrate that the condensation nuclei associated with a polluted atmosphere provide more favorable conditions than condensation nuclei associated with a clean atmosphere to produce dense advection fog, and that attaining a certain degree of supersaturation is not necessarily required for the formation of advection fog having condensation nuclei associated with a polluted atmosphere.

Hung, R. J.↗