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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 433 records · Page 24
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

State-selective probing of CO 2 autoionizing inner valence Rydberg states with attosecond extreme ultraviolet four-wave-mixing spectroscopy

Nonlinear spectroscopies can disentangle spectra that are congested due to inhomogeneous broadening. Here, in conjunction with theoretical calculations, attosecond extreme ultraviolet (XUV) four-wave-mixing (FWM) spectroscopy is utilized to probe the dynamics of autoionizing inner valence excited Rydberg states of the polyatomic molecule, CO 2 . This tabletop nonlinear technique employs a short attosecond XUV pulse train and two noncollinear, few-cycle near-infrared pulses to generate background-free XUV wave-mixing signals. FWM emission is observed from the n=5-7 states of the Henning sharp ndσ g Rydberg series that converges to the ionic $\widetilde{B}$ 2 Σ$^{+}_{u}$ state. However, these transient emission signals decay with lifetimes of 33 ± 6, 53 ± 2, and 94 ± 2 fs, respectively, which calculations show are consistent with the lifetimes of the short-lived n=6-8 members of the nsσ g character Henning diffuse Rydberg series. The oscillator strengths of transitions between states involved in all possible resonant FWM processes are calculated, verifying that the nonlinear spectra are dominated by pathways described by an initial excitation to the diffuse nsσ g Rydberg series and emission from the sharp ndσ g Rydberg series. The results substantiate not only that attosecond XUV FWM spectroscopy produces rigorous and meaningful measurements of ultrafast dynamics in polyatomic systems, but also that nonlinear spectroscopic techniques are versatile tools to selectively probe dynamics that are otherwise difficult to access.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Investigation on laser absorption and x-ray radiation in microstructured titanium targets heated by short-pulse relativistic laser pulses

The enhancement effect of a microstructured surface on laser absorption and characteristic K α emission has been investigated by measuring K-shell emission from titanium (Ti) targets irradiated with high-intensity ( ∼ 10 20 W cm − 2 ), subpicosecond (500 fs) laser pulses. The experimental results indicate a modest enhancement ( 1.6 × ) of K α emission from microstructured targets compared to flat foils, but with a similar intensity and profile of He α and Li-like satellites. Particle-in-cell (PIC) simulations are implemented to further understand the underlying physical processes in the laser interaction with both targets, interpreting the mechanisms responsible for the K α enhancement. The reasons for the lower-than-expected enhancement of K α emission are discussed. The rapid heating of the bulk plasma might result in the premature shutdown of K α emission before the thermalization of hot electrons or even the end of laser pulses, suggesting that the use of K α emission as a diagnostic of the hot-electron yield or relaxation could lead to a misinterpretation. Published by the American Physical Society 2024

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

A General Framework for Human-in-the-Loop Cognitive Digital Twins

Modelling and analysis of systems that are equipped with sensors and connected to the Internet are becoming more automated and less human-dependent. However, bringing expert knowledge into the loop along with data obtained from Internet of Thing (IoT) devices minimizes the risk of making poor and unexplainable decisions and helps to assess the impact of different strategies before applying them in reality. While Digital Twins are more of a data-driven simulation of the physical system, Cognitive Digital Twins bring the human dimension into the modelling and simulation. In this paper, we aim to emphasize the crucial role of explainability and the underlying rationale behind automated or interactive decision-making processes. Furthermore, we propose an initial framework that delineates the specific points within the feedback loop of a cognitive digital twin where human involvement can be incorporated.

Niloofar, Parisa↗
DOE OSTI2025

Deep potential molecular dynamics simulations of low-temperature plasma-surface interactions

Machine learning approaches to potential generation for molecular dynamics (MD) simulations of low-temperature plasma-surface interactions could greatly extend the range of chemical systems that can be modeled. Empirical potentials are difficult to generalize to complex combinations of multiple elements with interactions that might include covalent, ionic, and metallic bonds. This work demonstrates that a specific machine learning approach, Deep Potential Molecular Dynamics (DeepMD), can generate potentials that provide a good model of plasma etching in the Si-Cl-Ar system. Comparisons are made between MD results using DeepMD models and empirical potentials, as well as experimental measurements. Pure Si properties predicted by the DeepMD model are in reasonable agreement with experimental results. Simulations of Si bombardment by Ar + ions demonstrate the ability of the DeepMD method to predict sputtering yields as well as the depth of the amorphous-crystalline interface. Etch yields as a function of flux ratio and ion energy for simultaneous Cl 2 and Ar + impacts are in good agreement with previous simulation results and experiment. Predictions of etch yields and etch products during plasma-assisted atomic layer etching of Si-Cl 2 -Ar are shown to be in good agreement with MD predictions using empirical potentials and with experiment. Finally, good agreement was also seen with measurements for the spontaneous etching of Si by Cl atoms at 300 K. Further, the demonstration that DeepMD can reproduce results from MD simulations using empirical potentials is a necessary condition to future efforts to extend the method to a much wider range of systems for which empirical potentials may be difficult or impossible to obtain.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2025

Development and transferability of neural-network models for plasma-surface interactions

Plasma-surface interactions are increasingly critical to modern technologies; yet, accurate molecular dynamics simulations remain limited by the capabilities of interatomic potentials. Deep Potentials (DPs) promise to revolutionize the field by providing a systematic method for producing accurate interatomic potentials. The primary challenge of DP development is selecting a dataset, which efficiently spans the set of atomic environments one expects to encounter in the subsequent molecular dynamics simulations. The computational cost of density functional theory calculations, which are the typical basis for DP development, makes it impossible to directly verify the quality of a given DP. To address this challenge, we explore the development of a deep-learned interatomic potential, “DeepREBO,” trained to reproduce the behavior of the REBO2 empirical potential, enabling direct validation of training methodology and transferability. Using an active learning framework, we begin with a minimal dataset and iteratively expand it to train a Deep Potential-Smooth Edition model that faithfully reproduces REBO2 results for 25 eV hydrogen bombardment of diamond (001), a particularly challenging case. We show that small, carefully curated datasets can outperform large, unguided ones, with effective models requiring fewer than 15 000 snapshots. Subsequent transferability tests demonstrate that while DeepREBO generalizes well to diamond (111) surfaces, performance degrades for amorphous carbon or higher-energy impacts, highlighting the need for use-case-specific training data. We also evaluate methods to improve short-range repulsion. This study outlines best practices for training robust deep potentials and underscores the importance of dataset design for predictive plasma simulations.

Ab-initio molecular dynamics↗
DOE OSTI2023

Testing the contribution of dispersal to microbial succession following a wildfire

ABSTRACT Given increased wildfire activity, there is growing interest in understanding the drivers of microbial succession after fire. Dispersal may be especially important to post-fire succession as biotic communities can be more susceptible to invasion following a disturbance. Here, we experimentally manipulated dispersal into disturbed leaf litter communities collected following a wildfire and tracked bacterial and fungal dispersal assemblages over time. We show that the identity and source of microbes immigrating into the soil surface post-fire change across time with seasonal shifts and the reemergence of aboveground vegetation. Further, dispersal significantly contributed to the reassembly of leaf litter microbial communities after the fire, producing an increasingly distinct assembly trajectory. The effect of dispersal on α-diversity and β-diversity was ecosystem dependent but, unexpectedly, influenced bacterial and fungal communities in a similar manner within ecosystems. Collectively, these results demonstrate that dispersal explicitly alters the course of microbial community succession following a wildfire and may impact bacteria and fungi in parallel ways, despite differing in traits expected to alter dispersal patterns. IMPORTANCE Identifying the mechanisms underlying microbial community succession is necessary for predicting how microbial communities, and their functioning, will respond to future environmental change. Dispersal is one mechanism expected to affect microbial succession, yet the difficult nature of manipulating microorganisms in the environment has limited our understanding of its contribution. Using a dispersal exclusion experiment, this study isolates the specific effect of environmental dispersal on bacterial and fungal community assembly over time following a wildfire. The work demonstrates the potential to quantify dispersal impacts on soil microbial communities over time and test how dispersal might further interact with other assembly processes in response to environmental change.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

A Novel Method for Diagnosing Land–Atmosphere Coupling Sensitivity in a Single-Column Model

The response of boundary layer properties and cloudiness to changes in surface evaporative fraction (EF) is investigated in a single-column model to quantify the locally coupled impact of subgrid surface variations on the atmosphere during summer. Sensitive coupling days are defined when the model atmosphere exhibits large variations across a range of EFs centered on the analyzed value. Coupling sensitivity exists as both positive feedback (cloudiness increases with EF) and negative feedback (clouds increase with decreasing EF) regimes. The positive regime manifests in shallow convection situations, which are capped by a strengthened inversion and subsidence, restricting the vertical extent of convection to just above the boundary layer. Surfaces with larger EF (greater surface latent heat flux) can inject more moisture into the vertically confined system, lowering the cloud base and an increasing cloud liquid water path (LWP). Negative feedback regimes tend to manifest when large-scale deep convection, such as from mesoscale convective systems and fronts, is advected through the domain, where convection strengthens over surfaces with a lower EF (greater surface sensible heat flux). The invigoration of these systems by the land surface leads to an increase in LWP through strengthened updrafts and stronger coupling between the boundary layer and the free atmosphere. These results apply in the absence of heterogeneity-induced mesoscale circulations, providing a one-dimensional dynamical perspective on the effect of surface heterogeneity. Finally, this study provides a framework of intermediate complexity, lying between parcel theory and high-resolution coupled land–atmosphere modeling, and therefore isolates the relevant first-order processes in land–atmosphere interactions.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Kinetic effects of self-organization in low-temperature magnetized plasmas (Final Report for DE-SC0019045: 9/1/2018-8/31/2019)

The research goal of this Early Career Research Program project is to advance the science of low temperature magnetized plasmas using first-principles kinetic, e.g., solving the Boltzmann equation, models. A better understanding of the plasma transport properties, such as electrical resistivity and thermal conductivity must be obtained to better control and design magnetized plasma sources. A key physical phenomenon in low-temperature magnetized plasmas is the self-organization of plasma flows, e.g., coherent plasma structures and transition between different discharge modes. Understanding the physics of coherent plasma structures has been identified as one of the four important frontier topics in a recent workshop by the Office of Fusion Energy Science. These self-emerging plasma patterns results from the nonlinear coupling between plasma constituents (ions, electrons, and neutral atoms), electromagnetic fields, and materials. The physics of low-temperature magnetized plasmas is particularly complex because (i) the collisionless instabilities affect collisional phenomena (ionization, transport, etc.) and vice versa and (ii) the presence of materials (sheath, electron injection, etc.) influences the bulk plasma properties in low-temperature plasma (LTP) devices. Computational models of these plasma flows remain challenging because the plasma density can vary several orders of magnitudes, a wide range of temporal and spatial scales must be resolved, the phenomena are inherently three-dimensional, and various physical processes, such as wall interaction, instabilities, inelastic collisions, etc., must be simultaneously and self-consistently taken into account. Understanding the fundamental transport mechanisms in cross-field configurations enables additional controllability of plasma properties and electron energy distribution functions (EEDFs).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Amanzi–ATS: Modeling Environmental Systems across Scales [Brief]

Department of Energy national labs (Los Alamos, Oak Ridge, Lawrence Berkeley, and Pacific Northwest) designed Amanzi-ATS to model complex environmental systems across multiple scales. The open-source software includes the most complete suite of surface/subsurface processes, allowing users to select physical processes and their coupling interactions without rewriting software. Amanzi–ATS has been used to analyze pristine local watersheds, wildfire impact on watersheds, subsurface contaminant transport at legacy waste sites, the effect of a warming climate on the Arctic tundra, and groundwater in fractured porous media. Department of Energy national labs, U.S. Geological Survey, academia, and industry have applied the software.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Root Influences on Mobilization and Export of Mineral-bound Soil Organic Matter

Biogeochemical cycles within mountainous watersheds are key regulators of ecosystem carbon storage and downstream nutrient loadings, and they have shown to be particularly vulnerable to climate change impacts. Increasing temperature and persistent droughts have already dramatically changed vegetation cover across the mountainous western US, with unknown consequences for soil carbon and nutrient cycles belowground. What remains elusive is to what extent associated changes in root-soil interactions may mobilize the vast pool of organic matter (OM) that has been stabilized by associations with minerals for centuries or millennia. Although plant root-driven OM mobilization from minerals may be a central control on carbon loss and nutrient export, such mechanisms are currently missing from conceptual and numerical models. The overall objective of this Exploratory Project is to identify the biogeochemical mechanisms by which roots destabilize mineral-associated organic matter (MAOM) and the cumulative impact on carbon and nutrient fate. To accomplish this goal, we integrated well-controlled laboratory experiments with in-field measurements and a scalable modeling approach. First, we conducted model system experiments to assess the vulnerability of MAOM to exudate-mediated mechanisms. Our results show that common root exudates effectively destabilize MAOM not only through direct, ligand-driven mobilization mechanisms, but also indirect, microbially-mediated mechanisms relying on secondary metabolites and enzymes. We further found that OM bound to poorly crystalline Fe and Al (hydr)oxides is more vulnerable to exudate-induced destabilization than OM bound to more crystalline phases, particularly in response to direct, ligand-promoted mechanisms. These findings demonstrate that the stability of MAOM is not just a function of their inherent properties, but also will depend in large parts on the ability of plant roots and microbes to produce exudates capable of triggering suitable mobilization mechanisms. We further employed a well-controlled rhizobox approach, combining advanced microsensor and mass spectrometry techniques, to resolve spatiotemporal variations in the composition and availability of exudates along single growing roots of grasses. Our results show that the composition of functionally relevant exudate compounds varies at extremely short time scales, seemingly shifting from ligands such as aromatic acids around root tips to less reactive metabolites such as amino acids around mature root segments. These results suggest a prevalence of direct MAOM mobilization mechanisms around the root tip, while indirect MAOM mobilization strategies may dominate around more mature root segments. Additionally, we utilized microsensor measurements in rhizoboxes to parameterize a rhizosphere (hydro)biogeochemistry reactive transport model (eSTOMP-ROOTS). The resulting model was used to assess how root exudations affects the stability of MAOM. Model simulations show that diel pulses of root exudation are strong enough to cause oscillations in biogeochemical conditions—particularly in pH, oxygen concentrations, and microbial activity— that repeatedly disrupt MAOM. Finally, we assessed field-scale impacts of root-driven MAOM destabilization over short and long time scales. A combination of in-field incubations and field-based characterizations showed that MAOM may not only be vulnerable to seasonal variations in root activity, but also to root-driven weathering over pedogenic time scales. In sum, results from our Exploratory Award highlight the strong control plant roots exert on MAOM mobilization and, thus, on the potential for carbon and nutrient export from watersheds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2020

Conceptual Model Update of Mercury Sources and Flux at Y-12 and Upper East Fork Poplar Creek, Oak Ridge,Tennessee

The interactions between the key processes that control the fate and transport of mercury (Hg) in the sediments, groundwater, and stream water within the Y-12 National Security Complex (Y-12) in Oak Ridge, Tennessee are complex, and many aspects are not well understood. In contaminated environments such as Y-12, conceptual models are frequently developed to aid in visualizing and understanding the dynamic nature of the hydrologic, geochemical, and physical environment. These conceptual models integrate data in an internally consistent manner to understand processes that control the fate and transport of contaminants. Over the past few decades of environmental investigation at Y-12, a number of conceptual models have been developed to identify and define various technical processes at various scales. The main purpose of the activities described in this report is to update the 2011 conceptual model for Upper East Fork Poplar Creek using the most recent Hg concentration and flux data and informed scientific interpretation. Emphasis was placed on improving the previous model by implementing a more detailed spatial and temporal approach to visualize transport pathways in the watershed and trends in flux and concentration over time, and to compare baseflow and stormflow system dynamics. Detailed descriptions of historical and current Hg sources and transport pathways are also provided for the east and west ends of the facility. This conceptual model will allow the US Department of Energy to evaluate past and present remedial activities and provide a strong technical basis for prioritizing and optimizing remedial responses in a cost-effective and efficient manner. Twenty years ago, Hg flux from Outfall (OF) 200 at the headwaters of East Fork Poplar Creek represented approximately 20% of the overall flux leaving Y-12. By the time of the 2011 conceptual model report, that percentage had increased to 70%–80%. Flux estimates compiled for this report using data from 2009 to 2018 show that OF200 accounted for roughly 60% of the flux leaving Y-12. The relative role of the four storm drain conduits to OF200 appeared similar to 2011, with OF163 being the greatest contributor to downstream flux. An increase in Hg concentrations and flux occurred throughout and downstream of west end storm drains in 2011 in response to a storm drain cleanout. Leading up to the 2011 storm drain cleanout, annual baseflow flux was higher at OF200A6 than at Station 17. From 2011 to 2018, the trend reversed with concentrations and flux being higher at Station 17 than at OF200A6. A spike in concentrations occurred in July 2018, potentially due to a one-time influx of Hg that occurred during COLEX decontamination and decommissioning activities at Y-12. This report includes recommendations for improving our conceptual understanding of Hg sources, transport pathways, and flux at Y-12. Important recommendations include further evaluation of transport pathways, concurrent measurement of Hg concentration and flux under baseflow and stormflow conditions at multiple sites, and research to understand the connections among periphyton and methylmercury concentration, bioavailability, and bioaccumulation. Ongoing facility decontamination and decommissioning efforts, site characterization, remedial actions, and research are facilitating the collection of new Hg data at Y-12. The conceptual model update provided herein takes advantage of the extensive recent Hg sampling to provide an updated assessment of Hg mass balance and support a refined understanding of Hg behavior at or near Y-12. This assessment should assist in future environmental management decisions and in mitigating the impacts of Hg on the surrounding environment.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2022

Positive correlations between soil C stabilization and loss are regulated by roots, minerals, and microbes

Modern conceptual models of soil organic carbon (SOC) cycling place a strong focus on the microbe-mineral interactions that regulate C stabilization. However, the formation of ‘stable’ soil organic matter, which consists mainly of microbial residues bonded to mineral surfaces, is inextricably linked to C loss through microbial respiration. Therefore, what is the net impact of microbial metabolism on the total quantity of C held in the soil? To address this question, we constructed artificial root-soil systems to identify controls on C cycling across the plant-microbe-mineral continuum, simultaneously quantifying the formation of persistent mineral-associated C and C losses to respiration. Roots and minerals interacted to regulate these processes: while roots stimulated respiratory C losses and depleted mineral-associated C pools in low-activity clays, roots triggered formation of stable C in high-activity clays. Moreover, we observed a strong positive correlation between the formation of mineral-associated C and respiration. This suggests that the growth of persistent C pools which can resist subsequent disturbance comes at the expense of C loss from the system.

58 GEOSCIENCES↗
DOE OSTI2024

Investigation on laser absorption and x-ray radiation in microstructured titanium targets heated by short-pulse relativistic laser pulses

The enhancement effect of a microstructured surface on laser absorption and characteristic Kα emission has been investigated by measuring K-shell emission from titanium (Ti) targets irradiated with high-intensity (~10 20 W cm -2 ), subpicosecond (500 fs) laser pulses. The experimental results indicate a modest enhancement (1.6×) of Kα emission from microstructured targets compared to flat foils, but with a similar intensity and profile of Heα and Li-like satellites. Particle-in-cell (PIC) simulations are implemented to further understand the underlying physical processes in the laser interaction with both targets, interpreting the mechanisms responsible for the Kα enhancement. The reasons for the lower-than-expected enhancement of Kα emission are discussed. The rapid heating of the bulk plasma might result in the premature shutdown of Kα emission before the thermalization of hot electrons or even the end of laser pulses, suggesting that the use of Kα emission as a diagnostic of the hot-electron yield or relaxation could lead to a misinterpretation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Gasification of Coal/Plastic Mixtures: Fundamental Studies in a Laminar Entrained Flow Reactor

There is interest in leveraging entrained-flow coal gasification for co-processing plastic waste. However interactions between plastic and coal, particularly possible competition between coal volatiles and plastic vapors for oxygen, are not well understood. This study explores co-gasification of pulverized coal and plastic granules in a lab-scale entrained-flow reactor. Conversion and CO/CO2 ratio are given special attention.

Kareem, Afeez↗
DOE OSTI2026

Neutrinoless Double Beta Decay of 136 Xe and Related Nuclear Structure Studies (Final Scientific Report)

The search for neutrinoless double-beta decay (0nbb) explores new physics by directly probing the unknown mass scale and possible Majorana nature of the neutrino. The nEXO experiment, one of the two leading proposed ton-scale projects in the US, has a projected sensitivity to the 136 Xe 0nbb half-life of 10 28 years. The interpretation of possible signals in this next generation of experiments would be complicated by significant variations in theoretical calculations of the nuclear matrix elements (NMEs) of the decay, and nuclear structure measurements testing those theories can help address that uncertainty. We have 136 Xe(p,n) 136 Cs reaction at TUNL to deduce the level-scheme of states in 136 Cs through which the lowest-lying 1+ state decays. We find that over 99% of such decays will proceed through at least one isomeric state with a lifetime of order 100ns, which would enable large xenon detectors to employ a delayed-coincidence technique to search for charge-exchange processes including solar neutrino interactions. We have carried out measurements at TUNL of the 134 Xe( 3 He,n) 136 Ba and 136 Xe( 3 He,n) 138 Ba reactions to low-lying 0 + states in the residuals to probe the BCS assumption for QRPA NME calculations for the initial and final nuclei in 136 Xe 0nbb. While the analyses of these reactions is not yet complete and is ongoing, our initial results indicate tension with the BCS assumption. We have assembled a thermosyphon cooling R&D system for nEXO which has demonstrated up to 500 W of cooling in vacuum. We have developed a simple thermosyphon cooling simulation for nEXO and planned laboratory tests with the R&D system to benchmark it.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2023

Carbon stored in live ponderosa pines in the Sierra Nevada will not return to pre-drought (2012) levels during the 21st century due to bark beetle outbreaks

Outbreaks of several bark beetle species can develop rapidly in response to drought and may result in large transfers of carbon (C) stored in live trees to C stored in dead trees (10s of Tg C yr -1 in the western U.S. alone), which over time will be released back to the atmosphere. The western pine beetle (WPB) outbreak incited by the 2012–2015 mega-drought in the Sierra Nevada, California, U.S., could portend more frequent and/or severe bark beetle outbreaks as the temperature warms and drought frequency and intensity increase in the future. However, changes in the frequency and/or severity (resultant levels of host tree mortality) of beetle outbreaks are difficult to predict as outbreaks are complex with non-linear and eruptive processes primarily driven by interactions among beetle populations, the demography of hosts and other tree species, and climate and weather. Using an insect phenology and tree defense model, we projected the future likelihood of WPB outbreaks in the Sierra Nevada with climate drivers from different Earth System Models. Our goal was to understand how host (ponderosa pine, PIPO) recovery and future warming and drought affect the frequency and severity of WPB outbreaks and their C consequences. Our projections suggested that by 2100 the C stored in live PIPO (mean: 1.98 kg C m -2 , 95% CI: 1.74–2.21 kg C m -2 ) will not return to levels that occurred before the 2012–2015 drought (2012: ~2.30 kg C m –2 ) due to future WPB outbreaks. However, differences in climate models indicate a wide range of possible WPB outbreak frequencies and severities. Our results suggest that total plot basal area is the most significant factor in the mortality rate of PIPO by WPB in any given year, followed by drought severity and temperature. High levels of host basal area, higher temperature, and extreme drought all contribute to the frequency and severity of future WPB outbreaks. While PIPO basal area may decline under increased drought and warming, limiting high-stand basal area (>60 m 2 ha -1 ) may reduce the severity of future WPB outbreaks in the Sierra Nevada.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Vibronic Relaxation Pathways in Molecular Spin Qubit Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O under Pressure

In order to explore how spectral sparsity and vibronic decoherence pathways can be controlled in a model qubit system with atomic clock transitions, we combined diamond anvil cell techniques with synchrotron-based far infrared spectroscopy and first-principles calculations to reveal the vibrational response of Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O under compression. Because the hole in the phonon density of states acts to reduce the overlap between the phonons and f manifold excitations in this system, we postulated that pressure might move the HoO 4 rocking, bending, and asymmetric stretching modes that couple with the M J = ±5, ±2, and ±7 levels out of resonance, reducing their interactions and minimizing decoherence processes, while a potentially beneficial strategy for some molecular qubits, pressure slightly hardens the phonons in Na 9 [Ho(W 5 O 18 ) 2 ]·35H 2 O and systematically fills in the transparency window in the phonon response. The net result is that the vibrational spectrum becomes less sparse and the overlap with the various M J levels of the Ho 3+ ion actually increases. These findings suggest that negative pressure, achieved using chemical means or elongational strain, could further open the transparency window in this rare earth-containing spin qubit system, thus paving the way for the use of device surfaces and interface elongational/compressive strains to better manage decoherence pathways.

36 MATERIALS SCIENCE↗