Using bromide tracer to measure uranium diffusivity in ground water sediments

More than 129 million liters of groundwater are contaminated with uranium at Old Rifle, Colorado – a former uranium-processing site that operated until 1958. The original Department of Energy (DOE) strategy for remediation, involving natural flushing of U from the groundwater through mixing with surface water, has not proven successful. Thin pockets of silt-, clay-, and organic-rich sediments referred to as naturally reduced zones (NRZs) act both as sinks and sources of U to the aquifer, contribute to plume persistence, and appear to be diffusion limited controlled. To better understand how the NRZs are diffusion limited controlled, a bromide tracer was used to measure uranium diffusivity at two depths from the JB-02 well at Old Rifle: one depth in the middle of the NRZ and one depth at the bottom edge of the NRZ. A NaBr reservoir was allowed to diffuse into the sediments for several days with reservoir samples collected twice a day and analyzed using inductively coupled plasma mass spectrometry (ICP-MS) for bromide concentrations. This data was then used to calculate net flux, effective diffusivity, and the tortuosity effect within the sediments, which will inform uranium management strategies not only at the Old Rifle site but potentially other DOE legacy sites including Riverton, Wyoming and Shiprock, New Mexico

Element release and reaction-induced porosity alteration during shale-hydraulic fracturing fluid interactions

The use of hydraulic fracturing techniques to extract oil and gas from low permeability shale reservoirs has increased significantly in recent years. During hydraulic fracturing, large volumes of water, often acidic and oxic, are injected into shale formations. This drives fluid-rock interaction that can release metal contaminants (e.g., U, Pb) and alter the permeability of the rock, impacting the transport and recovery of water, hydrocarbons, and contaminants. To identify the key geochemical processes that occur upon exposure of shales to hydraulic fracturing fluid, we investigated the chemical interaction of hydraulic fracturing fluids with a variety of shales of different mineralogical texture and composition. Batch reactor experiments revealed that the dissolution of both pyrite and carbonate minerals occurred rapidly, releasing metal contaminants and generating porosity. Oxidation of pyrite and aqueous Fe drove precipitation of Fe(III)-(oxy)hydroxides that attenuated the release of these contaminants via co-precipitation and/or adsorption. The precipitation of these (oxy)hydroxides appeared to limit the extent of pyrite reaction. Enhanced removal of metals and contaminants in reactors with higher fluid pH was inferred to reflect increased Fe-(oxy)hydroxide precipitation associated with more rapid aqueous Fe(II) oxidation. The precipitation of both Al- and Fe-bearing phases revealed the potential for the occlusion of pores and fracture apertures, whereas the selective dissolution of calcite generated porosity. These pore-scale alterations of shale texture and the cycling of contaminants indicate that chemical interactions between shales and hydraulic fracturing fluids may exert an important control on the efficiency of hydraulic fracturing operations and the quality of water recovered at the surface

Multi-Messenger Gravitational Wave Searches with Pulsar Timing Arrays: Application to 3C66B Using the NANOGrav 11-year Data Set

When galaxies merge, the supermassive black holes in their centers may form binaries and, during the process of merger, emit low-frequency gravitational radiation in the process. In this paper we consider the galaxy 3C66B, which was used as the target of the first multi-messenger search for gravitational waves. Due to the observed periodicities present in the photometric and astrometric data of the source of the source, it has been theorized to contain a supermassive black hole binary. Its apparent 1.05-year orbital period would place the gravitational wave emission directly in the pulsar timing band. Since the first pulsar timing array study of 3C66B, revised models of the source have been published, and timing array sensitivities and techniques have improved dramatically. With these advances, we further constrain the chirp mass of the potential supermassive black hole binary in 3C66B to less than $(1.65\pm0.02) \times 10^9~{M_\odot}$ using data from the NANOGrav 11-year data set. This upper limit provides a factor of 1.6 improvement over previous limits, and a factor of 4.3 over the first search done. Nevertheless, the most recent orbital model for the source is still consistent with our limit from pulsar timing array data. In addition, we are able to quantify the improvement made by the inclusion of source properties gleaned from electromagnetic data to `blind' pulsar timing array searches. With these methods, it is apparent that it is not necessary to obtain exact a priori knowledge of the period of a binary to gain meaningful astrophysical inferences.Comment: 14 pages, 6 figures. Accepted by Ap

The NANOGrav 12.5-Year Data Set: Polarimetry and Faraday Rotation Measures from Observations of Millisecond Pulsars with the Green Bank Telescope

In this work, we present polarization profiles for 23 millisecond pulsars observed at 820 MHz and 1500 MHz with the Green Bank Telescope as part of the NANOGrav pulsar timing array. We calibrate the data using Mueller matrix solutions calculated from observations of PSRs B1929+10 and J1022+1001. We discuss the polarization profiles, which can be used to constrain pulsar emission geometry, and present both the first published radio polarization profiles for nine pulsars and the discovery of very low intensity average profile components ("microcomponents") in four pulsars. Using the Faraday rotation measures, we measure for each pulsar and use it to calculate the Galactic magnetic field parallel to the line of sight for different lines of sight through the interstellar medium. We fit for linear and sinusoidal trends in time in the dispersion measure and Galactic magnetic field and detect magnetic field variations with a period of one year in some pulsars, but overall find that the variations in these parameters are more consistent with a stochastic origin.Comment: 35 pages, 21 figures. Accepted to Ap

Bayesian Solar Wind Modeling with Pulsar Timing Arrays

Using Bayesian analyses we study the solar electron density with the NANOGrav 11-year pulsar timing array (PTA) dataset. Our model of the solar wind is incorporated into a global fit starting from pulse times-of-arrival. We introduce new tools developed for this global fit, including analytic expressions for solar electron column densities and open source models for the solar wind that port into existing PTA software. We perform an ab initio recovery of various solar wind model parameters. We then demonstrate the richness of information about the solar electron density, $n_E$, that can be gleaned from PTA data, including higher order corrections to the simple $1/r^2$ model associated with a free-streaming wind (which are informative probes of coronal acceleration physics), quarterly binned measurements of $n_E$ and a continuous time-varying model for $n_E$ spanning approximately one solar cycle period. Finally, we discuss the importance of our model for chromatic noise mitigation in gravitational-wave analyses of pulsar timing data and the potential of developing synergies between sophisticated PTA solar electron density models and those developed by the solar physics community.Comment: 22 pages, 7 figures, Submitted to Ap

An Unusual Pulse Shape Change Event in PSR J1713+0747 Observed with the Green Bank Telescope and CHIME

The millisecond pulsar J1713+0747 underwent a sudden and significant pulse shape change between 2021 April 16 and 17 (MJDs 59320 and 59321). Subsequently, the pulse shape gradually recovered over the course of several months. We report the results of continued multifrequency radio observations of the pulsar made using the Canadian Hydrogen Intensity Mapping Experiment and the 100 m Green Bank Telescope in a 3 yr period encompassing the shape change event, between 2020 February and 2023 February. As of 2023 February, the pulse shape had returned to a state similar to that seen before the event, but with measurable changes remaining. The amplitude of the shape change and the accompanying time-of-arrival residuals display a strong nonmonotonic dependence on radio frequency, demonstrating that the event is neither a glitch (the effects of which should be independent of radio frequency, ν) nor a change in dispersion measure alone (which would produce a delay proportional to ν−2). However, it does bear some resemblance to the two previous "chromatic timing events" observed in J1713+0747, as well as to a similar event observed in PSR J1643−1224 in 2015

An unusual pulse shape change event in PSR J1713+0747 observed with the Green Bank Telescope and CHIME

The millisecond pulsar J1713+0747 underwent a sudden and significant pulse shape change between April 16 and 17, 2021 (MJDs 59320 and 59321). Subsequently, the pulse shape gradually recovered over the course of several months. We report the results of continued multi-frequency radio observations of the pulsar made using the Canadian Hydrogen Intensity Mapping Experiment (CHIME) and the 100-meter Green Bank Telescope (GBT) in a three-year period encompassing the shape change event, between February 2020 and February 2023. As of February 2023, the pulse shape had returned to a state similar to that seen before the event, but with measurable changes remaining. The amplitude of the shape change and the accompanying TOA residuals display a strong non-monotonic dependence on radio frequency, demonstrating that the event is neither a glitch (the effects of which should be independent of radio frequency, $\nu$) nor a change in dispersion measure (DM) alone (which would produce a delay proportional to $\nu^{-2}$). However, it does bear some resemblance to the two previous "chromatic timing events" observed in J1713+0747 (Demorest et al. 2013; Lam et al. 2016), as well as to a similar event observed in PSR J1643-1224 in 2015 (Shannon et al. 2016).Comment: 19 pages, 8 figures. Submitted to ApJ. Data available at https://doi.org/10.5281/zenodo.723645

Multimessenger Gravitational-wave Searches with Pulsar Timing Arrays:Application to 3C 66B Using the NANOGrav 11-year Data Set

When galaxies merge, the supermassive black holes in their centers may form binaries and emit low-frequency gravitational radiation in the process. In this paper, we consider the galaxy 3C 66B, which was used as the target of the first multimessenger search for gravitational waves. Due to the observed periodicities present in the photometric and astrometric data of the source, it has been theorized to contain a supermassive black hole binary. Its apparent 1.05-year orbital period would place the gravitational-wave emission directly in the pulsar timing band. Since the first pulsar timing array study of 3C 66B, revised models of the source have been published, and timing array sensitivities and techniques have improved dramatically. With these advances, we further constrain the chirp mass of the potential supermassive black hole binary in 3C 66B to less than (1.65 ± 0.02) × 109 M o˙ using data from the NANOGrav 11-year data set. This upper limit provides a factor of 1.6 improvement over previous limits and a factor of 4.3 over the first search done. Nevertheless, the most recent orbital model for the source is still consistent with our limit from pulsar timing array data. In addition, we are able to quantify the improvement made by the inclusion of source properties gleaned from electromagnetic data over "blind"pulsar timing array searches. With these methods, it is apparent that it is not necessary to obtain exact a priori knowledge of the period of a binary to gain meaningful astrophysical inferences

The NANOGrav 11-year Data Set: High-precision Timing of 45 Millisecond Pulsars

We present high-precision timing data over time spans of up to 11 years for 45 millisecond pulsars observed as part of the North American Nanohertz Observatory for Gravitational Waves (NANOGrav) project, aimed at detecting and characterizing low-frequency gravitational waves. The pulsars were observed with the Arecibo Observatory and/or the Green Bank Telescope at frequencies ranging from 327 MHz to 2.3 GHz. Most pulsars were observed with approximately monthly cadence, and six high-timing-precision pulsars were observed weekly. All were observed at widely separated frequencies at each observing epoch in order to fit for time-variable dispersion delays. We describe our methods for data processing, time-of-arrival (TOA) calculation, and the implementation of a new, automated method for removing outlier TOAs. We fit a timing model for each pulsar that includes spin, astrometric, and (for binary pulsars) orbital parameters; time-variable dispersion delays; and parameters that quantify pulse-profile evolution with frequency. The timing solutions provide three new parallax measurements, two new Shapiro delay measurements, and two new measurements of significant orbital-period variations. We fit models that characterize sources of noise for each pulsar. We find that 11 pulsars show significant red noise, with generally smaller spectral indices than typically measured for non-recycled pulsars, possibly suggesting a different origin. A companion paper uses these data to constrain the strength of the gravitational-wave background