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DOE OSTI2025

Catalight─An Open-Source Automated Photocatalytic Reactor Package Illustrated through Plasmonic Acetylene Hydrogenation

An open-source and modular Python package, Catalight, is developed and demonstrated to automate (photo)catalysis measurements. (Photo)catalysis experiments require studying several parameters to evaluate performance, including the temperature, gas flow rate and composition, illumination power, and spectral profile. Catalight orchestrates measurements over this complicated parameter space and systematically stores, analyzes, and visualizes the results. To showcase the capabilities of Catalight, we perform an automated apparent activation barrier measurement of acetylene hydrogenation over a plasmonic AuPd catalyst on an Al 2 O 3 support, simultaneously varying laser power, wavelength, and temperature in a multiday experiment controlled by a simple Python script. Our chemical results unexpectedly show an increased activation barrier upon light excitation, contrary to previous findings for other plasmonic reactions and catalysts. We show that the reaction rate order with respect to both acetylene and hydrogen remains unchanged upon illumination, suggesting that molecular surface coverage is not changed by light. By analyzing the inhomogeneity of the laser-induced heating, we attribute these results to a partial photothermal effect combined with a photochemical/hot electron-driven mechanism. In conclusion, our findings highlight the capabilities of a new experiment automation tool; explore the photocatalytic mechanism for an industrially relevant reaction; and identify systematic sources of error in canonical photocatalysis experimental procedures.

Catalysts↗

DOE OSTI2018

COSMOGRAIL: the COSmological MOnitoring of GRAvItational Lenses: XVI. Time delays for the quadruply imaged quasar DES J0408–5354 with high-cadence photometric monitoring* [COSMOGRAIL XVI: Time delays for the quadruply imaged quasar DES J0408–5354 with high-cadence photometric monitoring]

Here, we present time-delay measurements for the new quadruple imaged quasar DES J0408–5354, the first quadruple imaged quasar found in the Dark Energy Survey (DES). Our result is made possible by implementing a new observational strategy using almost daily observations with the MPIA 2.2 m telescope at La Silla observatory and deep exposures reaching a signal-to-noise ratio of about 1000 per quasar image. This data qualityallows us to catch small photometric variations (a few mmag rms) of the quasar, acting on temporal scales much shorter than microlensing, and hence making the time delay measurement very robust against microlensing. In only seven months we very accurately measured one of the time delays in DES J0408–5354: Δt(AB) = –112.1 ± 2.1 days (1.8%) using only the MPIA 2.2 m data. In combination with data taken with the 1.2 m Euler Swiss telescope, we also measured two delays involving the D component of the system Δt(AD) = –155.5 ± 12.8 days (8.2%) and Δt(BD) = –42.4 ± 17.6 days (41%), where all the error bars include systematics. Turning these time delays into cosmological constraints will require deep Hubble Space Telescope (HST) imaging or ground-based adaptive optics (AO), and information on the velocity field of the lensing galaxy.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2014

Crosstalk elimination in the detection of dual-beam optical tweezers by spatial filtering

In dual-beam optical tweezers, the accuracy of position and force measurements is often compromised by crosstalk between the two detected signals, this crosstalk leading to systematic and significant errors on the measured forces and distances. This is true both for dual-beam optical traps where the splitting of the two traps is done by polarization optics and for dual optical traps constructed by other methods, e.g., holographic tweezers. If the two traps are orthogonally polarized, most often crosstalk is minimized by inserting polarization optics in front of the detector; however, this method is not perfect because of the de-polarization of the trapping beam introduced by the required high numerical aperture optics. Here we present a simple and easy-to-implement method to efficiently eliminate crosstalk. The method is based on spatial filtering by simply inserting a pinhole at the correct position and is highly compatible with standard back focal plane photodiode based detection of position and force. Our spatial filtering method reduces crosstalk up to five times better than polarization filtering alone. The effectiveness is dependent on pinhole size and distance between the traps and is here quantified experimentally and reproduced by theoretical modeling. The method here proposed will improve the accuracy of force-distance measurements, e.g., of single molecules, performed by dual-beam optical traps and hence give much more scientific value for the experimental efforts.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2020

Dark Energy Survey Identification of A Low-Mass Active Galactic Nucleus at Redshift 0.823 from Optical Variability

We report the identification of a low-mass active galactic nucleus (AGN), DES J0218−0430, in a redshift z = 0.823 galaxy in the Dark Energy Survey (DES) Supernova field. We select DES J0218−0430 as an AGN candidate by characterizing its long-term optical variability alone based on DES optical broad-band light curves spanning over 6 yr. An archival optical spectrum from the fourth phase of the Sloan Digital Sky Survey shows both broad Mg ii and broad H β lines, confirming its nature as a broad-line AGN. Archival XMM–Newton X-ray observations suggest an intrinsic hard X-ray luminosity of |$L_{{\rm 2-12\, keV}}\approx 7.6\pm 0.4\times 10^{43}$| erg s^−1, which exceeds those of the most X-ray luminous starburst galaxies, in support of an AGN driving the optical variability. Based on the broad H β from SDSS spectrum, we estimate a virial black hole (BH) mass of M_• ≈ 10^6.43–10^6.72 M_⊙ (with the error denoting the systematic uncertainty from different calibrations), consistent with the estimation from OzDES, making it the lowest mass AGN with redshift > 0.4 detected in optical. We estimate the host galaxy stellar mass to be M_* ≈ 10^10.5 ± 0.3 M_⊙ based on modelling the multiwavelength spectral energy distribution. DES J0218−0430 extends the M_•–M_* relation observed in luminous AGNs at z ∼ 1 to masses lower than being probed by previous work. Our work demonstrates the feasibility of using optical variability to identify low-mass AGNs at higher redshift in deeper synoptic surveys with direct implications for the upcoming Legacy Survey of Space and Time at Vera C. Rubin Observatory.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2018

The clustering of the SDSS-IV extended Baryon Oscillation Spectroscopic Survey DR14 quasar sample: structure growth rate measurement from the anisotropic quasar power spectrum in the redshift range 0.8 < z < 2.2

We analyse the clustering of the Sloan Digital Sky Survey IV extended Baryon Oscillation Spectroscopic Survey Data Release 14 quasar sample (DR14Q).We measure the redshift space distortions using the power-spectrum monopole, quadrupole, and hexadecapole inferred from 148 659 quasars between redshifts 0.8 and 2.2, covering a total sky footprint of 2112.9 deg 2 . We constrain the logarithmic growth of structure times the amplitude of dark matter density fluctuations, fσ 8 , and the Alcock–Paczynski dilation scales that allow constraints to be placed on the angular diameter distance D A (z) and the Hubble H(z) parameter. At the effective redshift of z eff = 1.52, fσ 8 (z eff ) = 0.420 ± 0.076, H(z eff ) = [162 ± 12] (r$fid\atop{s}$ /r s ) kms -1 Mpc -1 , and DA(z eff ) = [1.85 ± 0.11] × 10 3 (r s/ r$fid\atop{s}$) Mpc, where r s is the comoving sound horizon at the baryon drag epoch and the superscript ‘fid’ stands for its fiducial value. The errors take into account the full error budget, including systematics and statistical contributions. These results are in full agreement with the current Λ-Cold Dark Matter cosmological model inferred from Planck measurements. Finally, we compare our measurements with other eBOSS companion papers and find excellent agreement, demonstrating the consistency and complementarity of the different methods used for analysing the data.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Cohesion and excitations of diamond-structure silicon by quantum Monte Carlo: Benchmarks and control of systematic biases

We have carried out quantum Monte Carlo (QMC) calculations of silicon crystal focusing on the accuracy and systematic biases that affect the electronic structure characteristics. The results show that 64 and 216 atom supercells provide an excellent consistency for extrapolated energies per atom in the thermodynamic limit for ground, excited, and ionized states. We have calculated the ground state cohesion energy with both systematic and statistical errors below ≈ 0.05 eV. The ground state exhibits a fixed-node error of only 1.3(2)% of the correlation energy, suggesting an unusually high accuracy of the corresponding single-reference trial wave function. We obtain a very good agreement between optical and quasiparticle gaps that affirms the marginal impact of excitonic effects. Our most accurate results for band gaps differ from the experiments by about 0.2 eV. This difference is assigned to a combination of residual finite-size and fixed-node errors. In conclusion, we have estimated the crystal Fermi level referenced to vacuum that enabled us to calculate the edges of valence and conduction bands in agreement with experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2016

Cosmology with photometric weak lensing surveys: Constraints with redshift tomography of convergence peaks and moments

Weak gravitational lensing is becoming a mature technique for constraining cosmological parameters, and future surveys will be able to constrain the dark energy equation of state w. When analyzing galaxy surveys, redshift information has proven to be a valuable addition to angular shear correlations. We forecast parameter constraints on the triplet (Ω m ,w,σ 8 ) for a LSST-like photometric galaxy survey, using tomography of the shear-shear power spectrum, convergence peak counts and higher convergence moments. Here we find that redshift tomography with the power spectrum reduces the area of the 1σ confidence interval in (Ω m ,w) space by a factor of 8 with respect to the case of the single highest redshift bin. We also find that adding non-Gaussian information from the peak counts and higher-order moments of the convergence field and its spatial derivatives further reduces the constrained area in (Ω m ,w) by factors of 3 and 4, respectively. When we add cosmic microwave background parameter priors from Planck to our analysis, tomography improves power spectrum constraints by a factor of 3. Adding moments yields an improvement by an additional factor of 2, and adding both moments and peaks improves by almost a factor of 3 over power spectrum tomography alone. We evaluate the effect of uncorrected systematic photometric redshift errors on the parameter constraints. In conclusion, we find that different statistics lead to different bias directions in parameter space, suggesting the possibility of eliminating this bias via self-calibration.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Structure Factors of Neutron Matter at Finite Temperature

Here, we compute continuum and infinite volume limit extrapolations of the structure factors of neutron matter at finite temperature and density. Using a lattice formulation of leading-order pionless effective field theory, we compute the momentum dependence of the structure factors at finite temperature and at densities beyond the reach of the virial expansion. The Tan contact parameter is computed and the result agrees with the high momentum tail of the vector structure factor. All errors, statistical and systematic, are controlled for. This calculation is a first step towards a model-independent understanding of the linear response of neutron matter at finite temperature.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2022

Measurement of Compton Scattering at MAMI for the Extraction of the Electric and Magnetic Polarizabilities of the Proton

A precise measurement of the differential cross sections dσ/dΩ and the linearly polarized photon beam asymmetry Σ 3 for Compton scattering on the proton below pion threshold has been performed with a tagged photon beam and almost 4π detector at the Mainz Microtron. The incident photons were produced by the recently upgraded Glasgow-Mainz photon tagging facility and impinged on a cryogenic liquid hydrogen target, with the scattered photons detected in the Crystal Ball/TAPS setup. Using the highest statistics Compton scattering data ever measured on the proton along with two effective field theories (both covariant baryon and heavy-baryon) and one fixed-t dispersion relation model, constraining the fits with the Baldin sum rule, we have obtained the proton electric and magnetic polarizabilities with unprecedented precision: α E1 = 10.99 ± 0.16 ± 0.47 ± 0.17 ± 0.34, β M1 = 3.14 ± 0.21 ± 0.24 ± 0.20 ± 0.35; in units of 10 -4 fm 3 where the errors are statistical, systematic, spin polarizability dependent, and model dependent.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2014

Tolerance Studies of the Mu2e Solenoid System

The muon-to-electron conversion experiment at Fermilab is designed to explore charged lepton flavor violation. It is composed of three large superconducting solenoids, namely, the production solenoid, the transport solenoid, and the detector solenoid. Each subsystem has a set of field requirements. Tolerance sensitivity studies of the magnet system were performed with the objective of demonstrating that the present magnet design meets all the field requirements. Systematic and random errors were considered on the position and alignment of the coils. The study helps to identify the critical sources of errors and which are translated to coil manufacturing and mechanical support tolerances.

43 PARTICLE ACCELERATORS↗

DOE OSTI2014

SU-E-T-425: Spherical Dose Distributions for Radiosurgery Using a Standardized MLC Plan

Purpose: To investigate a standardized MLC treatment plan to generate small spherical dose distributions. Methods: The static virtual cone plan comprised six table positions with clockwise and counterclockwise arcs having collimator angles 45 and 135 degrees, respectively, at each position. The central two leaves of a 2.5 mm leaf width MLC were set to a constant gap. Control points were weighted proportional to the sine of the gantry angle. Plans were created for the 10 MV flattening-filter-free beam of a TrueBeam STx (Varian Medical Systems) with gaps of 1, 1.5, 2, and 3 mm and were delivered to a phantom containing radiochromic film. Dose was calculated using the Eclipse AAA (Varian Medical Systems). A dynamic plan in which the table and gantry moved simultaneously with 1.5 mm gap was also created and delivered using the TrueBeam developer mode. Results: The full-width-half-max (FWHM) varied with leaf gap, ranging from 5.2 to 6.2 mm. Calculated FWHM was smaller than measured by 0.7 mm for the 1 mm gap and ≤ 0.4 mm for the larger gaps. The measured-to-calculated dose ratio was 0.93, 0.96, 1.01, and 0.99 for 1 mm, 1.5 mm, 2 mm, and 3 mm gaps, respectively. The dynamic results were the same as the static. The position deviations between the phantom target position and the center of the dose distribution were < 0.4 mm. Conclusion: The virtual cone can deliver spherical dose distributions suitable for radio surgery of small targets such as the trigeminal nerve. The Eclipse AAA accurately calculates the expected dose, particularly for leaf gap ≥ 1.5 mm. The measured dose distribution is slightly larger than the calculation, which is likely due to systematic leaf position error, isocenter variation due to gantry sag and table eccentricity, and inaccuracy in MLC leaf end modeling.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2016

WE-AB-209-08: Novel Beam-Specific Adaptive Margins for Reducing Organ-At-Risk Doses

Purpose: Current practice of using 3D margins in radiotherapy with high-energy photon beams provides larger-than-required target coverage. According to the photon depth-dose curve, target displacements in beam direction result in minute changes in dose delivered. We exploit this behavior by generating margins on a per-beam basis which simultaneously account for the relative distance of the target and adjacent organs-at-risk (OARs). Methods: For each beam, we consider only geometrical uncertainties of the target location perpendicular to beam direction. By weighting voxels based on its proximity to an OAR, we generate adaptive margins that yield similar overall target coverage probability and reduced OAR dose-burden, at the expense of increased target volume. Three IMRT plans, using 3D margins and 2D per-beam margins with and without adaptation, were generated for five prostate patients with a prescription dose Dpres of 78Gy in 2Gy fractions using identical optimisation constraints. Systematic uncertainties of 1.1, 1.1, 1.5mm in the LR, SI, and AP directions, respectively, and 0.9, 1.1, 1.0mm for the random uncertainties, were assumed. A verification tool was employed to simulate the effects of systematic and random errors using a population size of 50,000. The fraction of the population that satisfies or violates a given DVH constraint was used for comparison. Results: We observe similar target coverage across all plans, with at least 97.5% of the population meeting the D98%>95%Dpres constraint. When looking at the probability of the population receiving D5<70Gy for the rectum, we observed median absolute increases of 23.61% (range, 2.15%–27.85%) and 6.97% (range, 0.65%–17.76%) using per-beam margins with and without adaptation, respectively, relative to using 3D margins. Conclusion: We observed sufficient and similar target coverage using per-beam margins. By adapting each per-beam margin away from an OAR, we can further reduce OAR dose without significantly lowering target coverage probability by irradiating more less-important tissues. This work is supported by Cancer Research UK under Programme C33589/A19908. Research at ICR is also supported by Cancer Research UK under Programme C33589/A19727 and NHS funding to the NIHR Biomedical Research Centre at RMH and ICR.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2016

TH-EF-BRA-11: Feasibility of Super-Resolution Time-Resolved 4DMRI for Multi-Breath Volumetric Motion Simulation in Radiotherapy Planning

Purpose: To develop a novel super-resolution time-resolved 4DMRI technique to evaluate multi-breath, irregular and complex organ motion without respiratory surrogate for radiotherapy planning. Methods: The super-resolution time-resolved (TR) 4DMRI approach combines a series of low-resolution 3D cine MRI images acquired during free breathing (FB) with a high-resolution breath-hold (BH) 3DMRI via deformable image registration (DIR). Five volunteers participated in the study under an IRB-approved protocol. The 3D cine images with voxel size of 5×5×5 mm{sup 3} at two volumes per second (2Hz) were acquired coronally using a T1 fast field echo sequence, half-scan (0.8) acceleration, and SENSE (3) parallel imaging. Phase-encoding was set in the lateral direction to minimize motion artifacts. The BH image with voxel size of 2×2×2 mm{sup 3} was acquired using the same sequence within 10 seconds. A demons-based DIR program was employed to produce super-resolution 2Hz 4DMRI. Registration quality was visually assessed using difference images between TR 4DMRI and 3D cine and quantitatively assessed using average voxel correlation. The fidelity of the 3D cine images was assessed using a gel phantom and a 1D motion platform by comparing mobile and static images. Results: Owing to voxel intensity similarity using the same MRI scanning sequence, accurate DIR between FB and BH images is achieved. The voxel correlations between 3D cine and TR 4DMRI are greater than 0.92 in all cases and the difference images illustrate minimal residual error with little systematic patterns. The 3D cine images of the mobile gel phantom preserve object geometry with minimal scanning artifacts. Conclusion: The super-resolution time-resolved 4DMRI technique has been achieved via DIR, providing a potential solution for multi-breath motion assessment. Accurate DIR mapping has been achieved to map high-resolution BH images to low-resolution FB images, producing 2Hz volumetric high-resolution 4DMRI. Further validation and improvement are still required prior to clinical applications. This study is in part supported by the NIH (U54CA137788/U54CA132378).

60 APPLIED LIFE SCIENCES↗

DOE OSTI2019

The strong coupling from $e^+e^-\to$~hadrons

We use a new compilation of the hadronic R R -ratio from available data for the process e^+e^-\to e + e − → hadrons below the charm mass to determine the strong coupling \alpha_s α s , using finite-energy sum rules. Quoting our results at the \tau τ mass to facilitate comparison to the results obtained from similar analyses of hadronic \tau τ -decay data, we find \alpha_s(m_\tau^2)=0.298\pm 0.016\pm 0.006 α s ( m τ 2 ) = 0.298 ± 0.016 ± 0.006 in fixed-order perturbation theory, and \alpha_s(m_\tau^2)=0.304\pm 0.018\pm 0.006 α s ( m τ 2 ) = 0.304 ± 0.018 ± 0.006 in contour-improved perturbation theory, where the first error is statistical, and the second error combines various systematic effects. These values are in good agreement with a recent determination from the OPAL and ALEPH data for hadronic \tau τ decays. We briefly compare the R(s) R ( s ) -based analysis with the \tau τ -based analysis.

Boito, Diogo↗

DOE OSTI2015

Muon Antineutrino Disappearance in the MINOS Experiment

Antineutrinos from the set of 7.09$\times 10^{20}$ Protons-on-target (POT) of $\nu_\mu\textrm{-dominant}$ and 3.40$\times 10^{20}$ POT of $\bar\nu_\mu\textrm{-enhanced}$ MINOS beam data is analysed to extract the antineutrino atmospheric-scale oscillation parameters $\left|\Delta\bar m^2\right|$ and $\sin^2\left(2\bar\theta\right)$. Using the Feldman-Cousins statistical technique to account for systematic and statistical errors, $\left|\Delta\bar m^2\right|=2.58^{+0.26}_{-0.17} \times 10^{-3}~\textrm{eV}^2$ and $\sin^2\left(2\bar\theta\right)=0.96^{+0.04}_{-0.10}$ were measured. This measurement of $\left|\Delta\bar m^2\right|$ improves on the previous world limits from Super-K by a factor of five. Any observed difference between the neutrino and antineutrino oscillation parameters could be an indication of CPT violation, or otherwise physics beyond the standard model. This measurement is consistent with the global limits on $\left|\Delta m^2\right|$ and $\sin^2\left(2\theta\right)$ for neutrinos.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2017

CPHASE gate with Rydberg atoms (CPHAR)

We demonstrate a controlled phase gate approach to entangling neutral atoms using a tunable, Rydberg-dressed interaction. Previous approaches utilize a “dipole blockade” or a “spin-flip blockade” and thereby lack arbitrary phase control, and are less extensible to simultaneous entangling operations in many-atom systems. We systematically study major error mechanisms that limit the fidelity of the entangling interaction and find the dominant error mechanism to be phase noise in the coherent control of the single spins. Our work charts a definitive path to high fidelity entanglement using Rydberg-state-mediated interactions in neutral atoms.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2019

Probabilistic Assembly of a Ball Screw

The assembly of ball screws is considered theoretically and experimentally in the case where the screw and nut are combined with an optimal combination of systematic and random errors in the screw pitch (optimal pitch error ratio).

42 ENGINEERING↗

DOE OSTI2017

The Physical Nature of Subdwarf A Stars: White Dwarf Impostors

We address the physical nature of subdwarf A-type (sdA) stars and their possible link to extremely low mass (ELM) white dwarfs (WDs). The two classes of objects are confused in low-resolution spectroscopy. However, colors and proper motions indicate that sdA stars are cooler and more luminous, and thus larger in radius, than published ELM WDs. We demonstrate that surface gravities derived from pure hydrogen models suffer a systematic ∼1 dex error for sdA stars, likely explained by metal line blanketing below 9000 K. A detailed study of five eclipsing binaries with radial velocity orbital solutions and infrared excess establishes that these sdA stars are metal-poor ≃1.2 M {sub ⊙} main sequence stars with ≃0.8 M {sub ⊙} companions. While WDs must exist at sdA temperatures, only ∼1% of a magnitude-limited sdA sample should be ELM WDs. We conclude that the majority of sdA stars are metal-poor A–F type stars in the halo, and that recently discovered pulsating ELM WD-like stars with no obvious radial velocity variations may be SX Phe variables, not pulsating WDs.

79 ASTRONOMY AND ASTROPHYSICS↗