Search NASA⌕ Search

Engineering topics

Paudel, Hari P.

Publications and source records attributed to Paudel, Hari P..

At least 19 records
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Quantum Sensing for Energy Applications

Quantum sensing is creating potentially transformative opportunities to exploit intricate quantum mechanical phenomena in new ways to make ultrasensitive measurements of multiple parameters. A growing interest in quantum sensing has created opportunities for its deployment to improve processes pertaining to energy production, distribution, and consumption. NETL is leveraging experimental and computational quantum tools to enhance sensitivity of hybrid quantum-classical ultrasensitive sensors for the detection of hydrocarbons and rare earth elements (REEs).

Paudel, Hari P.↗
DOE OSTI2024

Functionalization of nitrogen vacancy-containing nanodiamonds with a metal-organic framework for quantum sensing applications

Nitrogen vacancy (NV)-containing nanodiamonds (NDs) are an important material in applications such as biological imaging, catalysis, and, in particular, quantum sensing. Careful manipulation of the surface coating on NV NDs is essential for both enhancing quantum sensor performance and for tuning selectivity towards specific sensing targets. Here, we demonstrate a simple synthetic approach for functionalizing NV NDs with the zeolitic imidazole framework-8 (ZIF-8) metal–organic framework (MOF), providing a well-ordered, porous scaffold for immobilizing target analytes near the NV ND surface. The composites were structurally characterized by x-ray diffraction, electron microscopy, and X-ray photoelectron spectroscopy, and these results were all consistent with NV NDs fully encapsulated by ZIF-8. Critically, the luminescent properties of the NV NDs, which are vital for quantum sensing experiments such as optically detected magnetic resonance (ODMR), are unchanged by the MOF coating. Moreover, spin relaxometry experiments indicate that the ZIF-8 coating significantly enhances the NV ND spin longitudinal relaxation time T1, a critical quantum parameter for sensing applications. Given the tremendous structural diversity of MOFs, the NV ND@MOF composites are an exciting material class with exciting implications for the development of high-performance quantum sensors.

Crawford, Scott↗
DOE OSTI2024

First-Principles Studies of Tritium Species Diffusivity Across the Interface of Nickel-Plated Zircaloy-4

α-Zr and its alloys are known as best 3 H getters due to their excellent corrosion resistance under chemically corrosive environment, low thermal neutron absorption cross-section and robust mechanical strength at high temperature. In this work, we conducted a systematic study on constructing and optimizing Ni and Zr surfaces, interfacing the stable Ni and Zr surfaces to create an optimal Ni-Zr interface, and an understanding the diffusion mechanisms for 3 H across Ni(111)-Zr(0001) interface with and without vacancies and impurities such as Sn and O.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗
DOE OSTI2024

Assessing Ground State Energy of Molecules and Energy Profile of the NH3 Capturing CO2 System Using the Quantum Computing Algorithms

Molecule size correlates with the number of electrons on electronic energies and strength of anharmonicity on vibrational properties, however, it is challenging to address using classical computing. In this study, variational quantum eigensolver (VQE) algorithm was implemented on a quantum simulator to quantify electronic and vibrational energies and reaction pathways of CO2 + NH3 = NH2COOH. The VQE-based Hartree-Fock-Embedding algorithm was adopted to benchmark electronic energies for a series of molecules (doi.org/10.1063/5.0188249) and quantify the reaction energy profile of the CO2 capture reaction (doi.org/10.1116/5.0137750). The generated reaction profile is in good agreement with the classical high-level Coupled-Cluster-Singles-and-Doubles (CCSD) results. The quantum computing algorithm also helps enhance the calculation of vibrational ground-state energies by considering the many-body coupling using the Vibrational Self-Consistent Field method, providing results for CO2 and NH3 molecules with accuracy comparable to the direct diagonalization method. Our approach indicates quantum computing can be applied to solve practical problems.

Lee, Yueh-Lin↗
DOE OSTI2024

First-Principles Studies of Tritium Species Diffusivity Across the Interface of Nickel-Plated Zircaloy-4

In this study, we will calculate the 3H2 and 3H2O diffusion mechanism in the Ni coated layer and the dominant 3H species dissolution into the Zircaloy-4 getter. We will optimize the Ni/Zr interface and introduce Sn and O impurities. To achieve the objectives, we will perform the investigation by using spin-polarized density functional theory (DFT) methods to capture the effects of Ni magnetic properties on 3H diffusion. We will introduce NiO/Ni(OH) on the Ni side closer to the interface. Then, the 3H diffusion pathways and barriers from Ni side to the zircalory-4 will be explored. We will investigate how NiO/Ni(OH) affects the 3H diffusion across the interface.

Paudel, Hari P.↗
DOE OSTI2024

Factors that Impact the Redox Kinetics Associated with Sr1-xAxFeO3 (A = Ca, Ba) in Air Separations Technologies

Perovskite oxides, including SrFeO3-δ, have garnered significant interest for their impressive oxygen storage thermodynamics and kinetics. While traditional oxygen production is performed through cryogenic separation methods at the industrial scale, oxygen carrier-based separations have offered an attractive alternative at the modular scale. Perovskites are considered ideal oxygen carriers, with their structural flexibility minimizing both the thermodynamic barrier and the structural strain related to the oxygen uptake/release cycle. Our latest work has identified a few major factors that directly impact the oxygen release thermodynamics and kinetics for Sr1-xAxFeO3-δ (A = Ca, Ba) materials including elemental composition, crystallographic symmetry, surface area, and pretreatment conditions. This presentation will discuss these factors using Sr1¬-xCaxFeO3 and Ba1-xSrxFeO3 to illustrate their individual and collective impacts on the design of high-performance oxygen carriers when operating at 300-700 °C. Additionally, we will discuss how each of these factors can be leveraged for the numerous catalytic applications also dependent on the redox properties of mixed metal oxides.

Popczun, Eric↗
DOE OSTI2024

Quantum for Energy Systems and Technologies

Quantum Information Science (QIS) is expected to profoundly change the practice of science and engineering in the coming decades. QIS technology exploits quantum phenomena for performing tasks that are impossible to do today and is a rapidly progressing field, fueled by large investments from the private sector and governments. Its importance to the U.S. economy and national security is underscored by the National Quantum Initiative Act (NQIA) passed in December 2018, which creates a coordinated multiagency program to support research and training in QIS. After the NIQA signed into law, NETL has launched an initiative to apply QIS to problems encountered in energy technology development. In Jan. 2020, an Quantum for Energy Systems & Technologies (QUEST) working group was formed to establish a workforce capable of developing, reviewing, managing, and advising on QIS-related technologies for NETL and FECM. Since then, the QUEST team have been working on developing quantum sensing technology and performing quantum computing to solve energy-related problems. This poster summarized the QUEST team’s activities & accomplishments on QIS targeting energy-related applications.

Paudel, Hari P.↗
DOE OSTI2024

How Well Can Quantum Embedding Method Predict the Reaction Profiles for Hydrogenation of Small Li Clusters?

Quantum computing leverages the principles of quantum mechanics in novel ways to tackle complex chemistry problems that cannot be accurately addressed using traditional quantum chemistry methods. However, the high computational cost and available number of physical qubits with high fidelity limit its application to small chemical systems. This work employed a quantum-classical framework which features a quantum active space-embedding approach to perform simulations of chemical reactions that require up to 14 qubits. This framework was applied to prototypical example metal hydrogenation reactions: the coupling between hydrogen and Li 2 , Li 3 , and Li 4 clusters. Particular attention was paid to the computation of barriers and reaction energies. The predicted reaction profiles compare well with advanced classical quantum chemistry methods, demonstrating the potential of the quantum embedding algorithm to map out reaction profiles of realistic gas-phase chemical reactions to ascertain qualitative energetic trends. Additionally, the predicted potential energy curves provide a benchmark to compare against both current and future quantum embedding approaches.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Overview of Quantum Sensing Materials and Techniques for Energy Sector Applications

The energy sector is dependent upon highly sensitive sensing devices for a wide range of applications. Variables such as temperature, pH, electromagnetic fields, and pressure must be measured with high precision, often in harsh conditions (e.g. high temperature, pressure and humidity). These sensors are deployed in infrastructure such as transformers, pipelines, mines, nuclear power plants, and other areas to ensure safe operating conditions and uninterrupted, optimized service. Moreover, new opportunities for sensors have emerged due to the expansion of smart grids/meters, driverless vehicles, and the discovery of new oil/gas deposits. The continued maturation of quantum sensors offers exciting opportunities for quantum-enhanced measurements to improve sensitivity beyond the classical limit. Here, an overview of established and emerging quantum materials and methods for sensing applications will be provided. Opportunities within the energy sector for quantum sensors will then be analyzed, including oil/gas discovery, greenhouse gas emission monitoring, pH and ion sensing, current measurements, and quantum-enhanced spectroscopy, along with barriers such as quantum sensor platform miniaturization and ruggedization. A specific project at the National Energy Technology Laboratory involving the functionalization of qubits using metal-organic frameworks for enhanced quantum sensing will then be highlighted. Here, nitrogen vacancy centers (NV) in nanodiamonds, a commercially available qubit with long coherence times and utilizable quantum properties at room temperature, are encapsulated using the metal-organic framework ZIF-8. Significantly, the ZIF-8 coating increases the longitudinal spin relaxation lifetime of the NV centers, an important parameter for spin relaxometry-based quantum sensing experiments. These results demonstrate the importance of qubit functionalization as a crucial step for rationally designing high performance quantum sensors.

Crawford, Scott↗
DOE OSTI2024

Quantum Computing and Simulations for Energy Applications

While quantum computing (QC) is considered as a paradigm shift in our basic understanding of physical computation, effective implementation of QC in energy applications also depends on progress and development in the dimensions of both QC hardware and algorithms. To fully address the status and future challenges of QC applied within the energy sector, in this presentation, we firstly summarize recent advancements on the applications of QC to energy infrastructure and materials, complex energy system processes, advanced manufacturing, and energy system security. Then, we will demonstrate the results of QC performed both on a simulator and a quantum device targeting on energy-related applications.

Paudel, Hari P.↗
DOE OSTI2024

Magnetic Field Sensing via Optically Detected Magnetic Resonance and Spin Relaxometry Using Nitrogen Vacancies in Nanodiamonds

Quantum sensing is broadly defined as the use of quantum materials, quantum coherence, and/or quantum entanglement to measure physical quantities and/or to enhance the sensitivity of classical analytical measurements. Certain materials exhibit interesting quantum properties that have the potential to be utilized in quantum sensing applications. One such quantum property is electronic spin, which is utilized in this work. Here, we built a custom apparatus capable of conducting both optically detected magnetic resonance (ODMR) and spin relaxometry. The quantum material investigated was an ensemble of nitrogen vacancies (NV) in nanodiamonds. We have characterized the system and measured ODMR spectra for different strengths of the applied DC magnetic field and clearly observed the expected splitting of the resonances due to Zeeman splitting. We also have measured the spin relaxation times for two different powers of the applied AC magnetic field. The lower power dataset exhibited expected exponential temporal dependence of the relaxation of a modified spin state, whereas the higher power dataset exhibited stretched exponential dependence of the evolution of the modified spin state, indicating the presence of high-power phenomena that emerge that retard the relaxation of the spin state.

Lander, Gary↗
DOE OSTI2024

Magnetic Field Sensing via Optically Detected Magnetic Resonance and Spin Relaxometry Using Nitrogen Vacancies in Nanodiamonds

Quantum sensing is broadly defined as the use of quantum materials, quantum coherence, and/or quantum entanglement to measure physical quantities and/or to enhance the sensitivity of classical analytical measurements. Certain materials exhibit interesting quantum properties that have the potential to be utilized in quantum sensing applications. One such quantum property is electronic spin, which is utilized in this work. Here, we built a custom apparatus capable of conducting both optically detected magnetic resonance (ODMR) and spin relaxometry. The quantum material investigated was an ensemble of nitrogen vacancies (NV) in nanodiamonds. We have characterized the system and measured ODMR spectra for different strengths of the applied DC magnetic field and clearly observed the expected splitting of the resonances due to Zeeman splitting. We also have measured the spin relaxation times for two different powers of the applied AC magnetic field. The lower power dataset exhibited expected exponential temporal dependence of the relaxation of a modified spin state, whereas the higher power dataset exhibited stretched exponential dependence of the modified spin state, indicating the presence of high-power phenomena that emerge that retard the relaxation of the spin state.

Lander, Gary↗
DOE OSTI2024

Quantum for Energy Systems and Technologies

Quantum information science (QIS) is creating a transformative opportunity to improve processes for energy production, distribution, and consumption. In this presentation, we will show the works that are currently pursued into two major directions, (i) quantum sensing and (ii) quantum computing is undergoing in order to find applications in the areas of carbon captures, critical minerals and gas sensing applications.

Paudel, Hari P.↗
DOE OSTI2024

Sensing at the Nanoscale Using Nitrogen-Vacancy Centers in Diamond: A Model for a Quantum Pressure Sensor

The sensing of stress under harsh environmental conditions with high resolution has critical importance for a range of applications including earth’s subsurface scanning, geological CO2 storage monitoring, and mineral and resource recovery. Using a first-principles density functional theory (DFT) approach combined with the theoretical modelling of the low-energy Hamiltonian, here, we investigate a novel approach to detect unprecedented levels of pressure by taking advantage of the solid-state electronic spin of nitrogen-vacancy (NV) centers in diamond. We computationally explore the effect of strain on the defect band edges and band gaps by varying the lattice parameters of a diamond supercell hosting a single NV center. A low-energy Hamiltonian is developed that includes the effect of stress on the energy level of a ±1 spin manifold at the ground state. By quantifying the energy level shift and split, we predict pressure sensing of up to 0.3 MPa/Hz using the experimentally measured spin dephasing time. We show the superiority of the quantum sensing approach over traditional optical sensing techniques by discussing our results from DFT and theoretical modelling for the frequency shift per unit pressure. Importantly, we propose a quantum manometer that could be useful to measure earth’s subsurface vibrations as well as for pressure detection and monitoring in high-temperature superconductivity studies and in material sciences. Our results open avenues for the development of a sensing technology with high sensitivity and resolution under extreme pressure limits that potentially has a wider applicability than the existing pressure sensing technologies.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Ground state property calculations of LiH n complexes using IBM Qiskit’s quantum simulator

In this study, the variational quantum eigensolver (VQE) on a quantum simulator is used in calculating ground state electronic structure properties of the LiH n , n = 1–3, complexes including their singly charged ions. Results calculated using classical electronic structure algorithms are also included. We investigate the use of the unitary coupled cluster with singles and doubles (UCCSD) Ansatz using VQE within Qiskit and compare results to full configuration interaction (FCI) calculations. Computed ground state energies, electron affinities, ionization potentials, and dipole moments are considered. We report the first-of-its-kind simulated quantum computing results of selected LiH n species and use the parity orbital to qubit mapping scheme. We find that VQE/UCCSD results are comparable to classical coupled clusters with singles and doubles for all considered systems with respect to FCI. A VQE calculation cost evaluation is included in which we evaluate performance using both Jordan–Wigner and parity orbital to qubit mapping schemes. We also discuss some of the current limitations of utilizing VQE for the study of chemical systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2024

Ba₁₋ₓSrₓFeO₃₋ᵧ as an Improved Oxygen Carrier for Chemical Looping Air Separation: A Computational and Experimental Study

Chemical looping air separation (CLAS) is a promising method to generate pure carbon-dioxide from fuel combustion with a pure oxygen stream, which is produced through the capture, and targeted release, of oxygen from the atmosphere using a solid oxide carrier. The performance of this process depends on the redox characteristics of the oxide carrier. Using experimental oxygen-temperature-programmed desorption (TPD) and thermogravimetric analysis (TGA), the study shows that Ba₀․₇₅Sr₀․₂₅FeO₃ has improved oxygen storage capacity (OSC), oxidation, and reduction kinetics over pristine SrFeO₃ at temperatures ranging from 300-500 °C. The redox energetics computed by using first-principles density functional theory (DFT) calculations also depict the measured trend establishing it as an important descriptor of the measured performance. The Ba₁₋ₓSrₓFeO₃₋ᵧ depicts a Sr-substitution and oxygen stoichiometry induced structural phase transition from hexagonal at low temperatures to pseudo-cubic phase with higher OSC up to T=400 °C. Also, the mechanism leading to this structural phase transition is identified by performing electronic and vibrational structural calculations. This presentation was given on March 8, 2024 at the APS March Meeting in Minneapolis, MN.

Acharya, Shree Ram↗
DOE OSTI2024

Nitrogen Vacancy Centers in Diamond for Stress Sensing Applications: Theory and Experiments

Sensing of stress under high elevated environmental conditions with high resolution has critical importance for range of applications including earth’s subsurface scanning and geological CO2 storage monitoring. Using first principles density functional theory (DFT) approach combined with the theoretical modelling of low energy Hamiltonian, here we investigate a novel approach to detect unprecedented level of pressure by taking advantage of solid-state electron’s spin of Nitrogen vacancy (NV) centers in nanodiamond. We computationally explore the effect of strain on the defect band edges and band gaps by varying the lattice parameters of diamond supercell hosting a single NV center. A low energy Hamiltonian is developed that includes effect of stress on the energy level of ±1 spin manifold at the ground state. By quantifying the energy level shift and split, we predict the pressure sensing of up to 0.3 MPa/√Hz. We show superiority of the quantum sensing over traditional optical sensing techniques by discussing our results from DFT and theoretical modelling for the frequency shift per unit pressure. The proposed quantum stress sensing could be useful to measure earth’s subsurface vibrations. Our results open avenues for development of sensing technology with a high sensitivity and resolution under extreme pressure conditions that potentially has a wider applicability than existing pressure sensing technologies.

Paudel, Hari P.↗