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DOE OSTI2025

Atomic ionization: sd energy imbalance and Perdew–Zunger self-interaction correction energy penalty in 3d atoms

To accurately describe the energetics of transition metal systems, density functional approximations (DFAs) must provide a balanced description of s- and d- electrons. One measure of this is the sd transfer error, which has previously been defined as E ( 3 d n − 1 4 s 1 ) − E ( 3 d n − 2 4 s 2 ) . Theoretical concerns have been raised about this definition due to its evaluation of excited-state energies using ground-state DFAs. A more serious concern appears to be strong correlation in the 4s 2 configuration. Here, we define a ground-state measure of the sd energy imbalance, based on the errors of s- and d-electron second ionization energies of the 3d atoms, that effectively circumvents the aforementioned problems. We find an improved performance as we move from the local spin density approximation (LSDA) to the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation (GGA) to the regularized and restored Strongly Constrained and Appropriately Normed (r 2 SCAN) meta-GGA for first-row transition metal atoms. However, we find large (∼2 eV) ground-state sd energy imbalances when applying a Perdew–Zunger 1981 self-interaction correction. This is attributed to an “energy penalty” associated with the noded 3d orbitals. A local scaling of the self-interaction correction to LSDA results in a balance of s- and d-errors.

Science & Technology - Other Topics↗

DOE OSTI2020

Correlative electron and ion beam analysis of the electrochemical performances of LiV 3 O 8 cathode films as a function of microstructures

Degradation mechanisms in LiV 3 O 8 cathode films (~500 nm) with different initial microstructures i.e., globular nanocrystals in amorphous matrix and needle-like nanocrystals, synthesized by annealing the cathodes at 150 °C and 300 °C for 6 h are studied by Transmission Electron Microscopy (TEM) and Auger Electron Spectroscopy (AES). In addition, a unique in-situ combination of TEM and Secondary Ion Mass Spectrometry (SIMS) imaging techniques, namely Parallel Ion and Electron beam Spectrometry (PIES) is carried out to measure the 3D distribution of V and Li with nanoscale resolution. These characterization studies focus on correlating the pre- and post-cycling microstructure to observed electrochemical performance. The LiV 3 O 8 cathode film with needle-like nanocrystals (300 °C) shows a higher initial capacity but it degrades rapidly compared to the film with globular nanocrystals embedded in amorphous matrix (150 °C). We observed that LiV 3 O 8 films with needle-like nanocrystals are more susceptible to cathode decohesion and vanadium dissolution than the films with globular nanocrystals embedded in amorphous matrix, explaining the differences in their electrochemical performance. The findings from this study have relevance to the development of thin film electrode microstructures for high capacity and cyclic stability.

25 ENERGY STORAGE↗

DOE OSTI2023

Future precipitation increase constrained by climatological pattern of cloud effect

The fractional increase in global mean precipitation (?P ¯/P ¯) is a first-order measure of the hydrological cycle intensification under anthropogenic warming. However, ?P ¯/P ¯ varies by a factor of more than three among model projections, hindering credible assessments of the associated climate impacts. The uncertainty in ?P ¯/P ¯ stems from uncertainty in both hydrological sensitivity (global mean precipitation increase per unit warming) and climate sensitivity (global mean temperature increase per forcing). Here, by investigating hydrological and climate sensitivities in a unified surface-energy-balance perspective, we find that both sensitivities are significantly correlated with surface shortwave cloud feedback, which is further linked to the climatological pattern of cloud shortwave effect. The observed pattern of cloud effect thus constrains both sensitivities and consequently constrains ?P ¯/P ¯. The 5%-95% uncertainty range of ?P ¯/P ¯ from 1979-2005 to 2080-2100 under the high-emission (moderate-emission) scenario is constrained from 6.34±3.53% (4.19±2.28%) in the raw ensemble-model projection to 7.03±2.59% (4.63±1.71%). The constraint thus suggests a higher most-likely ?P ¯/P ¯ and reduces the uncertainty by ~25%, providing valuable information for impact assessments.

Zhou, Wenyu↗

DOE OSTI2022

Quantifying the Influence of Defects on Selectivity of Electrodes Encapsulated by Nanoscopic Silicon Oxide Overlayers

Encapsulation of electrocatalysts and photocatalysts with semipermeable nanoscopic oxide overlayers that exhibit selective transport properties is an attractive approach to achieve high redox selectivity. However, defects within the overlayers-such as pinholes, cracks, or particle inclusions-may facilitate local high rates of parasitic reactions by creating pathways for facile transport of undesired reactants to exposed active sites. Scanning electrochemical microscopy (SECM) is an attractive method to determine the influence of defects on macroscopic performance metrics thanks to its ability to measure the relative rates of competing electrochemical reactions with high spatial resolution over the electrode. Here, we report the use of SECM to determine the influence of overlayer defects on the selectivity of silicon oxide (SiOx) encapsulated platinum thin-film electrocatalysts operated under conditions where two competing reactions-the hydrogen evolution and Fe(III) reduction reactions-can occur. After an SECM methodology is described to determine spatially resolved selectivity, representative selectivity maps are correlated with the location of defects that are characterized by optical, electron, and atomic force microscopies. This analysis reveals that certain types of defects in the oxide overlayer are responsible for ∼60-90% of the partial current density toward the undesired Fe(III) reduction reaction. By correcting for defect contributions to Fe(III) reduction rates, true Fe(III) permeability values for the SiOxoverlayers were determined to be over an order of magnitude lower than permeabilities determined from analyses that ignore the presence of defects. Lastly, different types of defects were studied revealing that defect morphology can have varying influence on both redox selectivity and calculated permeability. This work highlights the need for spatially resolved measurements to evaluate the performance of oxide-encapsulated catalysts and understand their performance limits.

25 ENERGY STORAGE↗

DOE OSTI2025

Dynamical dark energy in light of the DESI DR2 baryonic acoustic oscillations measurements

Understanding whether cosmic acceleration arises from a cosmological constant or a dynamical component is a central goal of cosmology, and the Dark Energy Spectroscopic Instrument (DESI) enables stringent tests with high-precision distance measurements. Here we analyse measurements of baryon acoustic oscillations in DESI Data Release 1 and Data Release 2 and consider type Ia supernovae and a distance prior for the cosmic microwave background. With the larger statistical power and wider redshift coverage of Data Release 2, the preference for dynamical dark energy does not diminish relative to Data Release 1. Using both a shape-function reconstruction and non-parametric approaches with a Horndeski-motivated correlation prior, we find that the equation of state for dark energy w(z) varies with redshift. Baryon acoustic oscillation data alone yield modest constraints, but in combination with independent supernova compilations and the prior for the cosmic microwave background, they strengthen the evidence for dynamics. A Bayesian comparison of models shows moderate support for departures from Λ cold dark matter (ΛCDM) when several degrees of freedom in w(z) are allowed, corresponding to ~3σ tension with ΛCDM (and higher for some datasets). Despite methodological differences, our results are consistent with companion DESI papers, underscoring the complementarity of the approaches. Possible systematics remain under study; forthcoming DESI, Euclid and next-generation cosmic microwave background data will provide decisive tests.

cosmology↗

DOE OSTI2025

Dynamical dark energy in light of the DESI DR2 baryonic acoustic oscillations measurements

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2019

Pumped Storage Hydro Model Evaluation Report Task 1: Tool Assessment

Pumped storage hydro (PSH) projects support various aspects of power system operations. However, determining the value of PSH projects and the many services and contributions to the system they provide can be a challenge. The PSH techno-economic studies being carried out by a 5-lab consortium are defining extensive modeling approaches for evaluating the economic benefits of PSH projects. To enhance the impact of the valuation approach and follow-on techno-economic studies, Pacific Northwest National Laboratory (PNNL) will be developing a set of online tools that industry could adopt and use to advance PSH projects in the US. The problem is that the research team is not entirely clear on the features of the tools that would offer the most significant impact to industry. Thus, year one of this effort is designed to first define the needs of industry before developing the PSH valuation tool. The first step in defining industry needs is to evaluate existing tool packages, including those created by DOE and those by industry groups, to both measure usage levels and define tool attributes that maximize industry impact. The second step in this process will be to hold a workshop designed to elicit direct industry input. Given the breadth and nature of the task, which is to define ideal model attributes, the research team did not constrain the assessment to storage valuation tools. Several tools were assessed, and their characteristics compared against a list of “ideal” attributes that included ease of use, generalizability of results, and analytical flexibility. Information regarding usage and impact were then compared to specific model attributes to define which attributes appear to drive success. The following key lessons and implications can be drawn from the analysis: Models with high ease of use were often the most adopted by industry, though they did not necessarily have high publication reference records, meaning a published article made direct reference to the tool. For example, REScheck TM and COMcheck TM , two tools which share a site, have seen a high amount of web traffic and usage. Similarly, Storage Value Estimate Tool (StorageVET®), an energy storage valuation model, has a large number of organizations using it despite a low publication reference record. A common feature between these models is that they are web-hosted, theoretically making them more easily accessible with graphic user interfaces (GUIs) that are more navigable; Models with higher usage statistics were typically free and/or open source. While it may be unsurprising that this attribute could be considered a draw for users, there is the potential for overestimating the tool's value based on popularity due to the fact that some users may have used the model simply because it was free and not because it is the best model; Models that offer more in-depth analysis and a wide coverage of applications (e.g. VOLTTRON™, GridLAB-D™, and Integrated Valuation of Ecosystem Services and Tradeoffs (InVest)) have shown a high number of publication references as well as showing a high number of downloads in the case of GridLAB-D™. It should be noted that the figure below does not include the model with the highest number of publication references (EnergyPlus™) as it has been removed to show clearer distinction between the remaining tools; The most popular model within the evaluation list was EnergyPlus™. This tool has the highest number of publication references (2,034) of all models considered and contains both a high ease of use level as well as broad application flexibility. Its high usage may be correlated, however, with the presumed wider audience conducting energy consumption modeling compared to the audiences for some of the other tools in this list; Models that were low in both general usage and publication reference generally did not exhibit characteristics considered ideal by the research team. Some of these models offered a narrower range of analytical applications or lower generalizability of results. This would automatically restrict the pool of potential users to those who fall within a narrow range of specific technologies or applications. This report also explores two model structures for the PSH tool: decision tree-based, which would guide the user through the valuation methods defined in the PSH techno-economic studies currently being carried out by DOE, and an all-inclusive comprehensive model. The strengths of each were explored and a hybrid approach was defined that would embed a price taker model into the decision tree approach. Such an approach would provide a comprehensive approach for modeling small-scale PSH while recognizing the challenges associated with implementing a price-maker approach in an all-inclusive model. Insight gained in this analysis of other models can aid in narrowing down the list of effective and sought-after attributes, and in defining model structure. Next steps toward developing a model for storage valuation will be to gain direct industry input through workshops.

13 HYDRO ENERGY↗

DOE OSTI2025

Correlations between maximum mass of neutron stars and the nuclear matter properties and the constraints from PSR J0740+6620 and GW190814

The correlations between the maximum mass of neutron stars (NSs) with the properties of nuclear matter at saturation density ρ 0 , i.e., the incompressibility K 0 , the symmetry energy E sym (ρ 0 ), and its slope L(ρ 0 ), the isoscalar effective mass m$^{*}_{s0}$, and the parameter f I , have been investigated using several sets of Skyrme interactions based on the momentum-dependent (MD) Skyrme interactions SAMi-J27 (soft), SAMi-J31 (stiff), and SAMi-J35 (super-stiff), as well as the momentum-independent (MI) Skyrme interaction SkT5. Only one physical quantity is varied at a time for a given set of Skyrme interactions. It is found that the maximum mass of NSs has (1) a strong positive linear correlation with K 0 for stiff and super-stiff equation of state (EOS) and no correlation with K 0 for soft EOS; (2) a negative logarithm correlation with the symmetry energy E sym (ρ 0 ) for all the EOSs; (3) a positive logarithm correlation with the slope L(ρ 0 ) for all the EOSs; (4) a positive logarithm correlation with the parameter f I for MD EOS; (5) a negative power-law correlation with m$^{*}_{s0}$ for MD EOS. Based on these established correlations, the constraints to the nuclear matter properties from the mass of PSR J0740+6620 and GW190814 are investigated. Furthermore, we find that while rotation enhances the maximum mass of NSs, it does not effect the underlying correlations between the maximum mass and the aforementioned nuclear matter parameters.

Zhou, M. [Shaanxi Normal University, Xi’an (China)↗

DOE OSTI2025

Electron Energy-Loss Spectroscopy and Differential Phase Contrast Imaging with Active Decision in Multimodal Electron Microscopy: Isotopic detection at the atomic scale

Isotopic engineering provides a powerful route to control phonon behavior in crystalline solids, enabling fundamental studies of lattice dynamics and heat transport at the atomic scale. Here, we directly visualize isotope-dependent phonon propagation in epitaxial Cr 2 O 3 using aberration-corrected scanning transmission electron microscopy (STEM) combined with monochromated, high-energy-resolution electron energy-loss spectroscopy (EELS). Guided by ab initio phonon calculations, we demonstrate that optical phonon modes above 70 meV are predominantly oxygen-derived and exhibit measurable redshifts upon substitution of natural 16 O by enriched 18 O. Spatially resolved vibrational spectrum imaging reveals isotope-enriched tracer layers within Cr 2 O 3 thin films, correlating isotope concentration with phonon intensity variations and vibrational energy shifts. At the nanometer and atomic scales, vibrational EELS mapping uncovers coherent phonon propagation across isotopic interfaces, consistent with theoretical phonon density of states and dispersion relations. These results establish vibrational EELS as a quantitative probe for isotope-dependent phonon transport in materials, opening new possibilities for studying energy dissipation and lattice dynamics.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Tensile Deformation of DED Graded IN718-René41 Superalloy at 650°C by in-situ Neutron Diffraction and Digital Image Correlation

A compositionally graded material comprised IN718 (718, γ'/γ" strengthened superalloy) and René41 (R41, a medium γ' strengthened superalloy) was fabricated using laser blown-powder directed energy deposition (DED/LB-M). Hot gas path components that require high and low temperature capabilities at different locations may benefit from such graded superalloy, potentially eliminating the use of welded or mechanically joined components and reducing cost. In the present work, microstructure and 650°C tensile behavior of 718-R41 graded superalloy in as-built and heat-treated states are investigated by Digital Image Correlation (DIC), in-situ neutron diffraction, coupled with conventional characterization techniques. The applied heat treatment generates static recrystallization and equiaxed grains in 718 rich compositions, while R41 rich compositions remain partially or un-recrystallized. Yield strengths of 718 and R41 sections in heat-treated state are comparable to wrought forms but the graded compositions show weakness. From neutron experiment, diffraction elastic constants and single crystal elastic constants are calculated, which show small difference between the as-built and heat-treated states and between the γ and γ' phases. Grain-level load transfer from the (220) grains to (200) grains is found to be composition dependent, and qualitatively agrees with DIC measured macroscopic yield strength. Within the (200) grains, the γ/γ' phases deform elastically until the γ phase yields and afterwards the γ' phase takes load from γ phase.

digital image correlation↗

DOE OSTI2020

Relaxor behavior and electrothermal properties of Sn- and Nb-modified (Ba,Ca)TiO 3 Pb-free ferroelectric

Relaxor ferroelectrics have drawn attention for possible applications in solid-state cooling and thermal energy harvesting, owing to their electrothermal energy conversion properties. Here, we have synthesized and characterized the structure–property correlations of a new Sn- and Nb-doped (Ba,Ca)TiO 3 relaxor ferroelectric with large pyroelectric and electrocaloric effects over a broad temperature range. We observed two peaks for the temperature-dependent pyroelectric coefficient: (i) -(∂P/∂T) ~ 563 µC/(m 2 K) at T~ 270 K and (ii) -(∂P/∂T) ~ 1021 µC/(m 2 K) at T~ 320 K. In addition, a broad peak for electrocaloric temperature change is observed near 320 K with a relative cooling power of ~17 J/kg. These properties could be correlated to structural changes observed using X-ray diffraction at two different temperature ranges in the material. Analysis of high-energy X-ray scattering and specific heat capacity data revealed a transition from the cubic to tetragonal phase near T m ~ 320 K, whereas an additional increase in the tetragonality (c/a) of the polar phase is observed below T s ~ 270 K.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Dark Energy Survey Year 3 results: Measurement of the baryon acoustic oscillations with three-dimensional clustering

The three-dimensional correlation function offers an effective way to summarize the correlation of the large-scale structure even for imaging galaxy surveys. We have applied the projected three-dimensional correlation function, ξ p to measure the baryonic acoustic oscillations (BAO) scale on the first-three years Dark Energy Survey data. The sample consists of about 7 million galaxies in the redshift range 0.6< z p < 1.1 over a footprint of 4108 deg 2 . Our theory modeling includes the impact of realistic true redshift distributions beyond Gaussian photo-z approximation. ξ p is obtained by projecting the three-dimensional correlation to the transverse direction. To increase the signal-to-noise of the measurements, we have considered a Gaussian stacking window function in place of the commonly used top-hat. ξ p is sensitive to D M (z eff )/r s , the ratio between the comoving angular diameter distance and the sound horizon. Using the full sample, D M (z eff )/r s is constrained to be19.00 ± 0.67 (top-hat) and 19.15 ± 0.58 (Gaussian) at z eff = 0.835. The constraint is weaker than the angular correlation w constraint 18.84 ± 0.50), and we trace this to the fact that the BAO signals are heterogeneous across redshift. While ξ p responds to the heterogeneous signals by enlarging the error bar, w can still give a tight bound on D M s in this case. When a homogeneous BAO-signal subsample in the range 0.7 < z p <1.0 (z eff = 0.845) is considered, ξp yields 19.80 ± 0.67 (top-hat) and 19.84 ± 0.53 (Gaussian). The latter is mildly stronger than the w constraint (19.86 ± 0.55). We find that the ξ p results are more sensitive to photo-z because ξ p keeps the three-dimensional clustering information causing it to be more prone to photo-z noise. The Gaussian window gives more robust results than the top-hat as the former is designed to suppress the low signal modes. ξ p and the angular statistics such as w have their own pros and cons, and they serve an important crosscheck with each other.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2023

Origin and characterization of single-electron events in Skipper-CCDs for light dark matter searches

This manuscript summarizes the work carried out within the SENSEI (Sub-Electron-Noise Skipper-CCD Experimental Instrument) collaboration, an effort focused on the search for light dark matter using Skipper-CCDs. Firstly, it presents the data acquisition and processing protocol developed to establish a selection criteria for events compatible with the dark matter signal. This protocol also enabled the structure and tools used for the study and characterization of phenomena that impact the quality of measurements made in the search for dark matter (measurement of the Fano factor, determination of the Compton background, and characterization of the high-energy surface background), which were carried out during this work. Secondly, it discusses the comprehensive study conducted on the origin of single-electron events in Skipper-CCDs, which allowed for the selection of detector operating parameters and improved the detection sensitivity in the search for dark matter. It is highlighted the characterization of the spatial correlation between single-electron events and high-energy events, among other developed event selection criteria, and the optimization of the output device to reduce sources of luminescence during its operation. As a result of this study, the lowest levels of dark current and spurious charge ever measured in a CCD are reported. Finally, the latest published results from SENSEI are presented. The obtained limits for the scattering of a light mediator are the best reported to date across the entire investigated mass range, while for the heavy mediator, they are the best for masses below 10 MeV. In terms of dark matter absorption, the most restringent limits below 10 eV are reported. These results, achieved with only a very small fraction of the total projected exposure for SENSEI, position Skipper-CCDs as leaders in the search for light dark matter worldwide.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Effect of correlated oxide electrodes on disorder pinning and thermal roughening of ferroelectric domain walls in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films

We report the competing effects of disorder pinning and thermal roughening on ferroelectric domain walls as a function of temperature in epitaxial PbZr 0.2 Ti 0.8 O 3 thin films deposited on (001) SrTiO 3 substrates buffered by three types of correlated oxide electrodes, La 0.67 Sr 0.33 MnO 3 , LaNiO 3 , and SrIrO 3 . Piezo-response force microscopy studies show that the 50 nm PbZr 0.2 Ti 0.8 O 3 films are uniformly polarized in the as-grown states, with the patterned domain structures persisting above 700 °C. For all three types of films, the domain wall roughness is dominated by 2D random bond disorder at room temperature, and transitions to 1D thermal roughening upon heating. The roughness exponent ζ increases progressively from 0.3 to 0.5 within a temperature window that depends on the bottom conducting oxide type, from which we extracted the distribution of disorder pinning energy. Lastly, we discuss the possible origins of the disorder pinning and the effect of the correlated oxide electrodes on the energy landscape of DW motion.

36 MATERIALS SCIENCE↗

DOE OSTI2020

A complete grain-level assessment of the stress-strain evolution and associated deformation response in polycrystalline alloys

Polycrystalline alloys are used pervasively across structural applications contingent upon extensive experimental testing. A statistically representative number of tests are required to expose the variability in the material's performance, as a result of non-uniform microstructures and associated micromechanical fields. In a more direct means of capturing this pertinent information, multi-modal experimental techniques are presented to measure and track the complete micromechanical state, evolving during loading, of each and every grain within the regions of interest. Specifically, a combination of high-energy X-ray diffraction microscopy and digital image correlation coupled with electron backscatter diffraction are conducted on a specimen for each of the alloys, Haynes 282 and Ti7Al. The results of the multi-modal analysis definitively demonstrate that the degree of heterogeneity increases with deformation level and is used to assess the number of grains necessary for a representative volume element description of the stress state for each of these materials. Moreover, higher resolution imaging is used for identification of the slip system activity and subsequently used to study slip transmission events. An accurate knowledge of the resolved shear stress in adjacent grains (grain interactions) is demonstrated to be a key descriptor of the slip transmission events.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Elucidating Cycling Rate-Dependent Electrochemical Strains in Sodium Iron Phosphate Cathodes for Na-ion Batteries

Battery electrodes materials undergo significant mechanical instabilities which affects their longevity and exert rate-limitations during the cycling process. In this study, we investigate the rate-dependent mechanical response of sodium iron phosphate (NaFePO4, NFP) cathodes during Na intercalation via galvanostatic cycling at different rates by employing digital image correlation, electrochemical methods, and mathematical model. The mechanical behaviour of the electrode shows strong dependance on the applied scan rate. At slower rates, electrode shows asymmetrical strain generation between anodic and cathodic cycles, which is attributed to the formation of cathode-electrolyte interface layers. The electrode undergoes smaller strain generation when cycled at slower rates when the same amount of Na ions is removed or inserted into the electrode. A mathematical model was developed to predict strain evolution in the composite electrode as well as the concentration profile of the Na ions in the electrode particles. Rate-dependent and time dependent factors on the strain generation in the electrode are attributed to the capacity-dependent intercalation strains, rate-dependent mismatch strains, and time-dependent irreversible strains. The combination of in situ strain measurements with the analytical model provided new insight into the electrochemically induced mechanical deformations in Na-ion cathode electrodes.

Ozdogru, Bertan↗

DOE OSTI2020

Promoting the cleavage of C-O bonds at the interface between a metal oxide cluster and a Co(0001) support

As a first step toward the rational design of Co-based catalysts with a higher activity and selectivity, we determine how one can activate a C-O bond at the interface between a metal oxide cluster and a Co(0001) support. The hypothesis here is that the metal ions in metal oxide clusters on a Co(0001) support enhance the adsorption of CO and weaken the C-O bond strength, which can then facilitate the dissociation of the CO reactant. To test this hypothesis, we developed three computational models of Ti4O8/Co(0001), Zr4O8/Co(0001), and Mn8O8/Co(0001). We quantify the CO adsorption behavior at the interface sites between an oxide cluster and the Co(0001) support as well as the corresponding IR spectra. We correlate the computed CO stretch frequencies with their CO adsorption energies, as well as the CO stretch frequency with the C-O bond length, and related these findings to the changes in the chemical bonding in the bound CO. The interface is the most favorable site for CO adsorption. Adsorption results in an increase of the C-O bond length and a decrease in its vibrational frequency. From a chemical bonding analysis, the bond order in CO at this site drops from 3 (in the gas phase) to 1. This decrease in bond order is a necessary precursor stage for CO dissociation. The experimental measurements of the corresponding FTIR spectra support this point. The favorability of CO adsorption at the interface sites is due to an electron transfer from the metal ion in the metal oxide cluster to the O atom in CO. We establish a linear relationship between C-O bond length and CO frequency and this relationship is found to be independent of the support, type of metal oxide cluster, or the adsorption site.

Fischer-Tropsch Synthesis, Heterogeneous Catalysis↗

DOE OSTI2020

Identification of non-Fermi liquid fermionic self-energy from quantum Monte Carlo data

Quantum Monte Carlo (QMC) simulations of correlated electron systems provide unbiased information about system behavior at a quantum critical point (QCP) and can verify or disprove the existing theories of non-Fermi liquid (NFL) behavior at a QCP. However, simulations are carried out at a finite temperature, where quantum critical features are masked by finite-temperature effects. Here, we present a theoretical framework within which it is possible to separate thermal and quantum effects and extract the information about NFL physics at T = 0. We demonstrate our method for a specific example of 2D fermions near an Ising ferromagnetic QCP. We show that one can extract from QMC data the zero-temperature form of fermionic self-energy Σ(ω) even though the leading contribution to the self-energy comes from thermal effects. We find that the frequency dependence of Σ(ω) agrees well with the analytic form obtained within the Eliashberg theory of dynamical quantum criticality, and obeys ω 2/3 scaling at low frequencies. Our results open up an avenue for QMC studies of quantum critical metals.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗