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All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Measurement of double-differential charged-current Drell-Yan cross-sections at high transverse masses in $pp$ collisions at $\sqrt{s}$ = 13 TeV with the ATLAS detector

This paper presents a first measurement of the cross-section for the charged-current Drell-Yan process pp → W ± → ℓ ± ν above the resonance region, where ℓ is an electron or muon. The measurement is performed for transverse masses, $m$$^{W}_{T}$, between 200 GeV and 5000 GeV, using a sample of 140 fb −1 of pp collision data at a centre-of-mass energy of = 13 TeV collected by the ATLAS detector at the LHC during 2015–2018. The data are presented single differentially in transverse mass and double differentially in transverse mass and absolute lepton pseudorapidity. A test of lepton flavour universality shows no significant deviations from the Standard Model. The electron and muon channel measurements are combined to achieve a total experimental precision of 3% at low $m$$^{W}_{T}$. The single- and double differential W-boson charge asymmetries are evaluated from the measurements. A comparison to next-to-next-to-leading-order perturbative QCD predictions using several recent parton distribution functions and including next-to-leading-order electroweak effects indicates the potential of the data to constrain parton distribution functions. The data are also used to constrain four fermion operators in the Standard Model Effective Field Theory formalism, in particular the lepton-quark operator Wilson coefficient $c$$^{(c)}_{ℓq}$.

Hadron-Hadron Scattering↗
DOE OSTI2023

Measurement of $Z\gamma \gamma$ production in pp collisions at $\sqrt{s}= 13$ TeV with the ATLAS detector

Cross-sections for the production of a $Z$ boson in association with two photons are measured in proton–proton collisions at a centre-of-mass energy of 13 TeV. The data used correspond to an integrated luminosity of 139 fb -1 recorded by the ATLAS experiment during Run 2 of the LHC. The measurements use the electron and muon decay channels of the $Z$ boson, and a fiducial phase-space region where the photons are not radiated from the leptons. The integrated $Z$($\rightarrow$ $\ell$$\ell$)$\gamma \gamma$ cross-section is measured with a precision of 12% and differential cross-sections are measured as a function of six kinematic variables of the $Z\gamma \gamma$ system. The data are compared with predictions from MC event generators which are accurate to up to next-to-leading order in QCD. The cross-section measurements are used to set limits on the coupling strengths of dimension-8 operators in the framework of an effective field theory.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Measurements of Higgs boson production via gluon–gluon fusion and vector-boson fusion using $H\rightarrow WW^*\rightarrow \ell \nu \ell \nu$ decays in pp collisions with the ATLAS detector and their effective field theory interpretations

Higgs boson production cross-sections via gluon–gluon fusion and vector-boson fusion in proton–proton collisions are measured in the $H\rightarrow WW^*\rightarrow \ell \nu \ell \nu$ decay channel. The Large Hadron Collider delivered proton–proton collisions at a centre-of-mass energy of 13 TeV between 2015 and 2018, which were recorded by the ATLAS detector, corresponding to an integrated luminosity of $140\,\text {fb}^{-1}.$ The total cross-sections for Higgs boson production by gluon–gluon fusion and vector-boson fusion times the $H\rightarrow WW^*$ branching ratio are measured to be $12.4^{+1.3}_{-1.2}\,\text {pb}$ and $0.79^{+0.18}_{-0.16}\,\text {pb},$ respectively, in agreement with the Standard Model predictions. Higgs boson production is further characterised through measurements of Simplified Template Cross-Sections in a total of fifteen kinematic fiducial regions. A new scheme of kinematic fiducial regions has been introduced to enhance the sensitivity to CP-violating effects in Higgs boson interactions. Both schemes are used to constrain CP-even and CP-odd dimension-six operators in the Standard Model effective field theory.

Aad, G. [CPPM, Aix-Marseille Université, CNRS/IN2P↗
DOE OSTI2022

Scaling and adiabaticity in a rapidly expanding gluon plasma

In this work we aim to gain qualitative insight on the far-from-equilibrium behavior of the gluon plasma produced in the early stages of a heavy-ion collision. It was recently discovered [1] that the distribution functions of quarks and gluons in QCD effective kinetic theory (EKT) exhibit self-similar “scaling” evolution with time-dependent scaling exponents long before those exponents reach their pre-hydrodynamic fixed-point values. In this work we shed light on the origin of this time-dependent scaling phenomenon in the small-angle approximation to the Boltzmann equation. We first solve the Boltzmann equation numerically and find that time-dependent scaling is a feature of this kinetic theory, and that it captures key qualitative features of the scaling of hard gluons in QCD EKT. We then proceed to study scaling analytically and semi-analytically in this equation. We find that an appropriate momentum rescaling allows the scaling distribution to be identified as the instantaneous ground state of the operator describing the evolution of the distribution function, and the approach to the scaling function is described by the decay of the excited states. That is to say, there is a frame in which the system evolves adiabatically. Furthermore, from the conditions for adiabaticity we can derive evolution equations for the time-dependent scaling exponents. In addition to the known free-streaming and BMSS fixed points, we identify a new “dilute” fixed point when the number density becomes small before hydrodynamization. Corrections to the fixed point exponents in the small-angle approximation agree quantitatively with those found previously in QCD EKT and arise from the evolution of the ratio between hard and soft scales.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2021

CFD Simulation of Helium Flow Loop Test Section

A helium flow loop is being assembled at Oak Ridge National Laboratory to analyze heat transfer enhancement for systems such as blanket and divertor components. To efficiently identify optimum geometries for heat transfer enhancement in these applications, simulation work is performed to optimize test section designs that are built and tested in the helium flow loop that operates at 4 MPa and a mass flow rate of 100 g/s. Different ribbed geometries that examine rib shape, rib height, rib orientation, rib spacing, and three dimensional orientation are modeled and simulated in STAR-CCM+ to compare their ability to remove heat and mitigate pressure drop. Following the simulations, models are selected and manufactured for the helium flow loop tests. Simulations initially focus on a hydrodynamic study to determine the appropriate mesh and physics models and then add a heat flux to analyze the heat transfer abilities of the models. The simulations are run in steady state and use a Reynolds-averaged Navier-Stokes k-ε turbulence model. The helium is modeled as an ideal gas. The simulation explores models of geometries that enhance the heat transfer and decrease pressure drop with an overall goal of increasing fluid collision with the wall. Enhanced geometries are simulated to select appropriate designs for manufacturing, and preliminary experimental results are used to validate the simulations. Furthermore, the factors that are being analyzed in the comparison between the experimental and the simulated results include matching thermocouple temperatures, pressure drop, roughness, and fluid velocity.

42 ENGINEERING↗
DOE OSTI2024

Interpretive modeling of tungsten divertor leakage during experiments with neon gas seeding

Abstract Many existing and future tokamaks with tungsten divertors operate, or will operate, with low- Z impurity seeding, but the direct effect of these seeded impurities on tungsten Scrape-off-Layer (SOL) transport has not been explored in detail. This paper reports on a DIII-D experiment designed to test how tungsten divertor leakage from the Small-Angle Slot V-Shaped, tungsten-coated divertor is impacted by neon seeding at a variety of injection rates and poloidal injection locations. Measurements from the experiment show an inverse relationship between the neon injection rate and the tungsten core penetration factor. Interpretive modeling is performed with a combination of the SOLPS-ITER and DIVIMP codes to assess the underlying tungsten behavior. The modeling results show that the reduction in tungsten divertor leakage is driven by both an increase in the divertor collisionality as well as a reduction in the ion temperature gradient near the divertor target. Collisions between low- Z impurities and tungsten impurities are found to have a significant impact on the tungsten SOL transport, such that ignoring the low- Z impurity collisional effects on the tungsten transport can result in an overestimate of the divertor leakage by an order-of-magnitude. Given the importance of these localized interactions, neon seeding from the closed, slot-like divertor has a clear advantage in being able to reduce tungsten divertor leakage without the high levels of neon core contamination that occur when seeding from other poloidal locations.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Measurements of the pp → W ± γγ and pp → Zγγ cross sections at $ \sqrt{\mathrm{s}} $ = 13 TeV and limits on anomalous quartic gauge couplings

The cross section for W or Z boson production in association with two photons is measured in proton-proton collisions at a centre-of-mass energy of 13 TeV. The data set corresponds to an integrated luminosity of 137 fb -1 collected by the CMS experiment at the LHC. The W → ℓν and Z → ℓℓ decay modes (where ℓ = e, μ) are used to extract the Wγγ and Zγγ cross sections in a phase space defined by electron (muon) with transverse momentum larger than 30 GeV and photon transverse momentum larger than 20 GeV. All leptons and photons are required to have absolute pseudorapidity smaller than 2.5. The measured cross sections in this phase space are σ(Wγγ) = ${13.6}_{-1.9}^{+1.9}{\left(\mathrm{stat}\right)}_{-4.0}^{+4.0}$ (syst) ± 0.08 (PDF + scale) fb and σ(Zγγ) = ${5.41}_{-0.55}^{+0.58}{\left(\mathrm{stat}\right)}_{-.070}^{+0.64}$(syst) ± 0.06 (PDF + scale) fb. Limits on anomalous quartic gauge couplings are set in the framework of an effective field theory with dimension-8 operators.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Physics Guided Simulation of Electrostatic Discharge: Technical Report

Triboelectrically-charged objects may create threshold sparks, electrostatic discharge (ESD) events, to equilibrate charge between themselves and other relatively charged objects. ESD events exhibit many complex physical phenomena. They are a nexus of several fields of physics with disparate characteristic scales: plasma physics, chemical kinetics, hydrodynamics, circuit models, etc. These scales can span many orders of magnitude from the varied collisions thermalizing information within a plasma on the $\mathcal{O}(fs/ps)$ to the physical size of the plasma channel on the $\mathcal{O}(100µm)$, to the speed of a nonlinear hydrodynamic wave propagating at $\mathcal{O}(µm, ns)$. These threshold ESD events may occur in situations of programmatic importance, delivering energy and power profiles to a “victim load” generating deleterious consequences. To predict and mitigate these consequences we must answer questions about the spark’s energy budget: how much energy goes into producing the spark channel; how much gets radiated away; how much energy is advected away into the hydrodynamics; and how much energy is delivered to a victim load. An ESD simulation toolset has been created and evolved in order to answer these questions. An appropriate, physics guided implementation for simulation can be done by gaining insight into its constituent physics and leveraging that intuition to choose a suitable numerical operator. We examine in detail the chemical kinetics, circuit discharge, and hydrodynamics to deter mine dominant regimes, values, timescales, and interactions to uncover the underlying physical dynamics. We also examine and propose model reduction schemes for high-dimensional chemical kinetics. We use past and current work with experimentally validated and theoretically-verified hydrodynamics to calculate applicability limits of the non-ionizing strong shock limit. We quantify the energy budget from a hydrodynamic perspective and demonstrate that a significant fraction of the stored energy is “earmarked” for hydrodynamic advection as an energy terminus. Lastly, we combine the constituent physics of an ESD event (chemical kinetics, circuit model, and hydrodynamics) into a cohesive, actionable toolset and obtain promising results from an isothermal test case. We then propose a viable, modular evolution of the ESD toolset based upon the performed examination of the physics uncovering dominant physical scales and the stiffness of the compositional differential system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Measurements of differential cross-sections in top-quark pair events with a high transverse momentum top quark and limits on beyond the Standard Model contributions to top-quark pair production with the ATLAS detector at $ \sqrt{s} $ = 13 TeV

Cross-section measurements of top-quark pair production where the hadronically decaying top quark has transverse momentum greater than 355 GeV and the other top quark decays into ℓνb are presented using 139 fb –1 of data collected by the ATLAS experiment during proton-proton collisions at the LHC. The fiducial cross-section at √s = 13 TeV is measured to be σ = 1.267 ± 0.005 ± 0.053 pb, where the uncertainties reflect the limited number of data events and the systematic uncertainties, giving a total uncertainty of 4.2%. The cross-section is measured differentially as a function of variables characterizing the tt¯ system and additional radiation in the events. The results are compared with various Monte Carlo generators, including comparisons where the generators are reweighted to match a parton-level calculation at next-to-next-to-leading order. The reweighting improves the agreement between data and theory. The measured distribution of the top-quark transverse momentum is used to search for new physics in the context of the effective field theory framework. No significant deviation from the Standard Model is observed and limits are set on the Wilson coefficients of the dimension-six operators O tG and $O$ $^{(8)}_{tq}$, where the limits on the latter are the most stringent to date.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Search for heavy Majorana neutrinos in e ± e ± and e ± μ ± final states via WW scattering in pp collisions at s = 13 TeV with the ATLAS detector

A search for heavy Majorana neutrinos in scattering of same-sign W boson pairs in proton–proton collisions at $\sqrt{s}$ = 13 TeV at the LHC is reported. The dataset used corresponds to an integrated luminosity of 140 fb -1 , collected with the ATLAS detector during 2015–2018. The search is performed in final states including a same-sign ee or eμ pair and at least two jets with large invariant mass and a large rapidity difference. No significant excess of events with respect to the Standard Model background predictions is observed. The results are interpreted in a benchmark scenario of the Phenomenological Type-I Seesaw model. New constraints are set on the values of the |V eN | 2 and |V eN V$^{*}_{μN}$| parameters for heavy Majorana neutrino masses between 50 GeV and 20 TeV, where V ℓN is the matrix element describing the mixing of the heavy Majorana neutrino mass eigenstate with the Standard Model neutrino of flavour ℓ = e,μ. The sensitivity to the Weinberg operator is investigated and constraints on the effective ee and eμ Majorana neutrino masses are reported. The statistical combination of the ee and eμ channels with the previously published μμ channel is performed.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Measurement of the cross section for electroweak production of a Z boson, a photon and two jets in proton-proton collisions at $\sqrt{s} =$ 13 TeV and constraints on anomalous quartic couplings

A measurement is presented of the cross section for electroweak production of a Z boson and a photon in association with two jets (Zγjj) in proton-proton collisions. The Z boson candidates are selected through their decay into a pair of electrons or muons. The process of interest, electroweak Zγjj production, is isolated by selecting events with a large dijet mass and a large pseudorapidity gap between the two jets. The measurement is based on data collected at the CMS experiment at $ \sqrt{s} $ = 13 TeV, corresponding to an integrated luminosity of 35.9 fb$^{−1}$. The observed significance of the signal is 3.9 standard deviations, where a significance of 5.2 standard deviations is expected in the standard model. These results are combined with published results by CMS at $ \sqrt{s} $ = 8 TeV, which leads to observed and expected respective significances of 4.7 and 5.5 standard deviations. From the 13 TeV data, a value is obtained for the signal strength of electroweak Zγjj production and bounds are given on quartic vector boson interactions in the framework of dimension-eight effective field theory operators.[graphic not available: see fulltext]

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Physics Opportunities at a Beam Dump Facility at PIP-II and Beyond

The accelerator complex at Fermilab is currently undergoing improvements which will increase the available beam power to the complex and is known as Proton Improvement Plan-II (PIP-II). The PIP-II Linac is slated for operation near the end of this decade and will be the main proton driver for Fermilab experiments moving forward and provide the beam to LBNF/DUNE. However, the DUNE physics program requires only ~1% of the available protons provided by PIP-II. The Accelerator Complex Enhancement, or ACE, will provide further up grades in the 2030s in the form of increased power to LBNF along with a replacement for the Fermilab Booster which could also include an accumulator ring. A workshop was recently held at Fermilab in order to explore the physics possible when PIP-II is coupled with a fixed target or beam dump. The beam dump scenario pro vides an exciting opportunity to search for dark sector physics across detector threshold energy scales with examples being accelerator-produced dark matter, active-to-sterile neutrino oscillations, millicharged parti cles, and axion-like particles, which can be produced in the proton collisions with a fixed target. Additionally, experiments located at a PIP-II facility that is coupled to an accumulator ring would also be able to study coherent elastic neutrino-nucleus scattering, or CEvNS. In this talk, I will summarize the physics possible at a PIP-II beam dump facility and sensitivities to different dark sector physics and other beyond the Standard Model searches with detector concepts spanning from an eV-scale to MeV-scale detection threshold.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Developing and Evaluating a Smart Curtailment Strategy Integrated with a Wind Turbine Manufacturer Platform

The Renewable Energy Wildlife Institute lead a team of scientists, wind developers, and turbine manufacturers in a study to develop and test a “smart curtailment” system intended to help reduce bat collisions with wind turbines. The Vestas Bat Protection System (VBPS) is a newly developed software module within the Supervisory Control and Data Acquisition (SCADA) system of Vestas turbines. The VBPS combines data from commercially available environmental sensors and the turbine’s built-in sensors with the Vestas SCADA system. VBPS is designed to receive environmental data from sensors on the turbine such as temperature, wind speed, wind direction, time of day, and time of year, relays that information to the SCADA system to determine whether to execute turbine curtailments at any given time. The goals of this study were to 1) develop a bat fatality risk model based on bat activity data and environmental data collected in year 1, and to 2) evaluate the VBPS, using the bat fatality risk model to implement curtailment, in comparison to “blanket curtailment” (turbines curtailed when wind speed is below 5.0 meters per second (m/s)) and “control” (normally operating, feathered below 3.0 m/s) turbines in year 2. The field study took place at a wind energy facility in Iowa during the fall bat migration seasons (July – October) in 2021 and 2022. For VBPS to succeed as a viable strategy for the minimization of bat fatalities, it should meet or exceed the performance of blanket curtailment. Specifically, the VBPS should meet the following performance targets to demonstrate whether it an effective, practical risk reduction measure: (1) Turbines operating VBPS should have equal or fewer bat fatalities compared to turbines operating with blanket curtailment, and significantly fewer bat fatalities compared to control turbines; and (2) Turbines operating VBPS should have greater power production compared to turbines operating with blanket curtailment. The study was completed in accordance with the Statement of Project Objectives and within the terms of the Budget Justification. This Final Report describes the progress, challenges, and outcomes of the study.

17 WIND ENERGY↗
DOE OSTI2025

Observation of VVZ production at $\sqrt{s}$ = 13 TeV with the ATLAS detector

A search for the production of three massive vector bosons, VVZ(V = W, Z) , in proton-proton collisions at $\sqrt{s}$ = 13 TeV is performed using data with an integrated luminosity of 140 fb -1 recorded by the ATLAS detector at the Large Hadron Collider. Events produced in the leptonic final states WWZ → ℓvℓvℓℓ (ℓ = e,μ), WZZ → ℓvℓℓℓℓ, ZZZ → ℓℓℓℓℓ, and the semileptonic final states WWZ → qq ℓvℓℓ and WZZ → ℓv qq ℓℓ, are analysed. The measured cross section for the pp → VVZ process is 660$^{+93}_{-90}$(stat.)$^{+80}_{-81}$(syst.) fb, and the observed (expected) significance is 6.4 (4.7) standard deviations, representing the observation of VVZ production. In addition, the measured cross section for the pp → WWZ process is 442 ± 94(stat.)$^{+60}_{-52}$(syst.) fb, and the observed (expected) significance is 4.4 (3.6) standard deviations, representing evidence of WWZ production. The measured cross sections are consistent with the Standard Model predictions. Constraints on physics beyond the Standard Model are also derived in the effective field theory framework by setting limits on Wilson coefficients for dimension-8 operators describing anomalous quartic gauge boson couplings.

Aad, G. (ORCID:0000000266654934)↗
DOE OSTI2022

Measurement of the energy asymmetry in $t\bar{t} j$ production at 13 TeV with the ATLAS experiment and interpretation in the SMEFT framework

A measurement of the energy asymmetry in jet-associated top-quark pair production is presented using 139fb -1 of data collected by the ATLAS detector at the Large Hadron Collider during pp collisions at $\sqrt{s}$ =13TeV. The observable measures the different probability of top and antitop quarks to have the higher energy as a function of the jet scattering angle with respect to the beam axis. The energy asymmetry is measured in the semileptonic $t\bar{t}$ decay channel, and the hadronically decaying top quark must have transverse momentum above 350GeV. The results are corrected for detector effects to particle level in three bins of the scattering angle of the associated jet. The measurement agrees with the SM prediction at next-to-leading-order accuracy in quantum chromodynamics in all three bins. In the bin with the largest expected asymmetry, where the jet is emitted perpendicular to the beam, the energy asymmetry is measured to be -0.043 ± 0.020, in agreement with the SM prediction of -0.037 ± 0.003. Interpreting this result in the framework of the Standard Model effective field theory (SMEFT), it is shown that the energy asymmetry is sensitive to the top-quark chirality in four-quark operators and is therefore a valuable new observable in global SMEFT fits.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Observation of four-top-quark production in the multilepton final state with the ATLAS detector

This paper presents the observation of four-top-quark ($t$$\overline{t}$$t$$\overline{t}$) production in proton-proton collisions at the LHC. The analysis is performed using an integrated luminosity of 140 fb -1 at a centre-of-mass energy of 13 TeV collected using the ATLAS detector. Events containing two leptons with the same electric charge or at least three leptons (electrons or muons) are selected. Event kinematics are used to separate signal from background through a multivariate discriminant, and dedicated control regions are used to constrain the dominant backgrounds. The observed (expected) significance of the measured $t$$\overline{t}$$t$$\overline{t}$ signal with respect to the standard model (SM) background-only hypothesis is 6.1 (4.3) standard deviations. The $t$$\overline{t}$$t$$\overline{t}$ production cross section is measured to be ${22.5}^{+6.6}_{-5.5}$, consistent with the SM prediction of 12.0 ± 2.4 fb within 1.8 standard deviations. Data are also used to set limits on the three-top-quark production cross section, being an irreducible background not measured previously, and to constrain the top-Higgs Yukawa coupling and effective field theory operator coefficients that affect $t$$\overline{t}$$t$$\overline{t}$ production.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2025

Evaluating Movement Patterns of the Rattlesnake Hills Elk Herd on Hanford for Calendar Years 2019-2024

Biologists first documented elk on the Hanford Site in 1972; since then, the elk herd known as the Rattlesnake Hills Elk Herd (RHEH) has grown substantially (PNNL-13331, Population Characteristics and Seasonal Movement Patterns of the Rattlesnake Hills Elk Herd: Status Report 2000). Through the 1990s, the core range of the RHEH was focused on the portion of the Hanford Reach National Monument known as the Fitzner-Eberhardt Arid Lands Ecology (ALE) Reserve. More recently, larger numbers of elk have been occupying the U.S. Department of Energy (DOE), Hanford Field Office (HFO), formerly the DOE, Richland Operations Office managed portion- of the Hanford Site, known as central Hanford (Figure 1-1). This began with bachelor groups of bulls occupying the site intermittently, and the herd has grown to resident herds, including bulls, cows, and calves. The Washington Department of Fish and Wildlife (WDFW) established a target herd size for the RHEH of less than 350 animals to minimize damages on adjacent private agricultural lands (Washington State Elk Herd Plan–Yakima Elk Herd [WDFW 2002]). Attempts to control the RHEH population through hunting on private lands and a relocation effort during 2000 have failed to limit growth of the population toward the WDFW target, and the herd exceeds 1,600 according to recent counts (PNNL-13331; DOE/RL- 2023-20, Hanford Annual Site Environmental Report for Calendar Year 2022). Although elk are present on central Hanford year-round, they continue to move between areas offsite, the ALE Reserve, and central Hanford throughout the year, and it is these movements that result in many of the elk-vehicle collisions (EVC) that occur along Hanford Site roads and on the Washington State highways bordering the site. In addition, changes in management strategies on the ALE Reserve, including recent and potential future tribal elk hunts, may alter herd behavior and result in additional animals transiting onto and off central Hanford.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2026

Mechanistic Insights for Plasma-Catalytic CO 2 Reduction over TiO 2 in a Dielectric Barrier Discharge Reactor

Reaction kinetics experiments coupled with phenomenological kinetic modeling and parameter estimation are used to elicit insights into the mechanism and active sites for the plasma-catalytic dissociation of CO 2 on TiO 2 . Experimental and model insights showed that gas-phase reactions contribute at least two-thirds of the overall product formation at explored conditions; weak temperature dependence, strong sensitivity to specific energy input (SEI), apparent first order in CO 2 , and positive influence of cofed argon (Ar) and oxygen (O 2 ) for the gas-phase contributions all suggest that expected plasma reaction steps such as electron-impact and high-energy collisions are the dominant modes for CO 2 dissociation. The Arrhenius-like expression for gas contributions resulted in a preexponential of 4.40 × 10 –3 s –1 , an E SEI,g of 7.90 × 10 –4 mol/kJ, and an E a,g of 1.00 × 10 –3 J/mol. For surface contributions, the small apparent barrier of 16.3 kJ/mol, relatively weaker dependence on SEI, first-order dependence on CO 2 , and insensitivity to cofed Ar and O 2 all point to CO 2 dissociation on TiO 2 surface facets without vacancies and aided by plasma (leading to vibrationally excited CO 2 and/or a reactive surface with significant surface charge accumulation). The Arrhenius-like expression resulted in a preexponential of 7.81 × 10 –2 s –1 , an E SEI,s of 1.90 × 10 –3 mol/kJ, and an E a,s of 1.63 × 10 4 J/mol. The derived kinetic model further enabled a systematic evaluation of the effect of inputs (plasma power, flow rate, CO 2 inlet concentration, and temperature) to identify process trends and optimal operating conditions.

catalyst↗