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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 73 records · Page 4
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Optical Interference for the Guidance of Cryogenic Focused Ion Beam Milling Beyond the Axial Diffraction Limit

Using a tri-coincident cryogenic FIB-SEM-LM system, we identify an interferometric optical response that can be used for targeting lamella production to fluorescently labelled structures with accuracy beyond the diffraction limit. We demonstrate the approach using synthetic samples of fluorescent beads embedded in micron-scale droplets of water. Here, we then apply the approach to capture virions inside host cells. Successful targeting is confirmed by cryogenic electron tomography revealing clusters of virions in intracellular vesicles.

Sica, Anthony V. [SLAC National Accelerator Labora↗
DOE OSTI2023

Electric Field Analysis in a Cold-Ion Source Using Stark Spectroscopy of Rydberg Atoms

Here, we analyze electric fields in ion sources generated by quasicontinuous photoionization of cold Rb atoms trapped in the focal spot of a near-concentric, in-vacuum cavity for 1064-nm laser light. Ion streams are extracted with an external electric field, F. Stark effects of Rb 57F and of nearby high-angular-momentum Rydberg levels, which exhibit large, linear Stark shifts, are employed to study the net electric-field probability distribution within the ion-source region over an extraction-field range of 0 < F < 0.35 V/cm. For F = 0, we also investigate ion-field-induced Stark spectra of the 60P 1/2 state, which exhibits a (lesser) quadratic electric-field response that affords a simplified electric-field analysis. Experimental Rydberg spectra are compared with theoretical Stark spectra, which are weighted with net electric-field distributions obtained from classical ion-trajectory simulations that include Coulomb interactions. Experiments and models are in good agreement. At small F and high ion-source rates, the field approximately follows a Holtsmark distribution, and the ion streams are degraded by the Coulomb microfields. With increasing F and at lower ion-source rates, the fields become narrowly distributed around F, resulting in directional ion streams that are less degraded by microfields. Our results are of interest for monitoring cold-ion sources for focused-ion-beam applications, where Coulomb interactions are of concern, and for studies of electric fields in cold plasmas.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Electronic and optical properties of Zn-doped β-Ga 2 O 3 Czochralski single crystals

β-Ga 2 O 3 has several soluble deep acceptors that impart insulating behavior. In this study, we investigate Zn doping (0.25at.%) in bulk Czochralski and vertical gradient freeze β-Ga 2 O 3 . Representative crystals were assessed for orientation (electron backscatter diffraction and Raman spectroscopy), purity (glow discharge mass spectrometry and secondary ion mass spectrometry), optical properties (ultraviolet to near infrared absorption), and electrical properties (resistivity and current–voltage). Purity measurements indicate that Zn evaporation is insufficient to inhibit doping of Zn into β-Ga 2 O 3 . Hybrid functional calculations show Zn substitutes nearly equally on tetrahedral and octahedral sites, with less than ~0.1eV preference for the octahedral (Ga II ) site. Furthermore, calculations show that Zn Ga acts as a deep acceptor with trapping levels ~1.3 and ~0.9eV above the valence band for one and two holes, respectively. The solubility and electronic behavior of Zn dopants are consistent with measured concentrations >1×10 18 atoms/cm 3 and electrical measurements that show resistivity 10 11 –10 13 Ωcm, with no p-type conduction.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Synthetic Absorption Lines from Simulations of Multiphase Gas in Galactic Winds

Supernova-driven galactic winds are multiphase streams of gas that are often observed flowing at a range of velocities out of star-forming regions in galaxies. In this study, we use high-resolution 3D simulations of multiphase galactic winds modeled with the hydrodynamics code Cholla to investigate the connection between numerical studies and observations. Using a simulated interaction between a hot $T$ ~ 10 4 K supernova-driven wind and a cool $T$ ~ 10 7 K cloud of interstellar material, we create mock observables, including the optical depth ($\tau$) and covering fraction ($C$ $f$ ) of six commonly observed ions (Si II , C II , Si IV , C IV , N V , and O VI ) as a function of gas velocity. We compare our mock observables to surveys of galactic winds in the literature, finding good agreement with velocities and profiles of the low ions. We then compute "empirical" values for the optical depth and covering fraction following observational techniques and compare them to the values calculated directly from the simulation data. We find that the empirically computed values tend to underestimate the "true" value of $\tau$ for ions with high optical depth and overestimate the "true" value of $\tau$ for ions with low optical depth relative to the simulated data. In conclusion, the empirically estimated covering fractions match our direct calculations very well for the low-ionization ions; for the high-ionization ions, the empirical covering fractions underestimate the directly computed values by up to ~40%.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

The Dynamical Role of Optical Phonons and Sublattice Screening in a Solid-State Ion Conductor

Solid-state electrolytes (SSEs) require ionic conductivities that are competitive with liquid electrolytes to realize applications in all-solid-state batteries. Although candidate SSEs have been discovered, the underlying mechanisms enabling superionic conduction (>1 mS cm –1 ) remain elusive. In particular, the role of ultrafast lattice dynamics in mediating ion migration, which involves couplings between ions, phonons, and electrons, is rarely explored experimentally at their corresponding time scales. To investigate the complex contributions of coupled lattice dynamics on ion migration, we modulate the charge density occupations within the crystal framework and then measure the time-resolved change in impedance on picosecond time scales for a candidate SSE, Li 0.5 La 0.5 TiO 3 (LLTO). Upon perturbation, we observe enhanced ion migration at ultrafast time scales. The respective transients match the time scales of optical and acoustic phonon vibrations, suggesting their involvement in ion migration. We further computationally evaluate the effect of a charge transfer from the O 2p to the Ti 3d band on the electronic and physical structure of LLTO. We hypothesize that the charge-transfer excitation distorts the TiO 6 polyhedra by altering the local charge density occupancy of the hopping site at the migration pathway saddle point, thereby causing a reduction in the migration barrier for the Li + hop. We rule out the contribution of photogenerated electron carriers and laser heating. Overall, our investigation introduces a new spectroscopic tool to probe fundamental ion hopping mechanisms transiently at ultrafast time scales, which has previously only been achieved in a time-averaged manner or solely via computational methods.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Toroidal plasma acceleration due to NBI fast ion losses in LTX- β

The recent Lithium Tokamak Experiment-Beta (LTX- β ) upgrade includes the addition of neutral beam injection (NBI) in the same direction as the plasma current (co- I P ) and a new toroidal Mirnov array for MHD characterization. In initial NBI experiments, a spontaneously rotating n = 1 MHD mode is seen to accelerate during NBI in the counter-beam direction, accompanied by a rise in electron density consistent with the beam-injected inventory but without a clear increase in plasma pressure. Together with analytic and numerical modeling of beam optics and fast ion confinement, these observations indicate the prompt loss of all or nearly all beam ions. However, the same modeling also suggests that planned upgrades to the Ohmic heating system should provide the fast ion confinement necessary for beam heating and core fueling. Here, a simple analytic model relates the momentum confinement time τ Φ to the observed evolution of mode rotation due to the combination of NBI momentum coupling, fast ion loss $\vec{J}\times\vec{B}$, and anomalous viscous torques, yielding τ Φ values consistent with past measurements of electron energy confinement time τ E,e .

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Quasi-deterministic localization of Er emitters in thin film TiO 2 through submicron-scale crystalline phase control

With their shielded 4f orbitals, rare-earth ions (REIs) offer optical and electron spin transitions with good coherence properties even when embedded in a host crystal matrix, highlighting their utility as promising quantum emitters and memories for quantum information processing. Among REIs, trivalent erbium (Er 3+ ) uniquely has an optical transition in the telecom C-band, ideal for transmission over optical fibers, making it well suited for applications in quantum communication. The deployment of Er 3+ emitters into a thin film TiO 2 platform has been a promising step toward scalable integration; however, like many solid-state systems, the deterministic spatial placement of quantum emitters remains an open challenge. Here, we investigate laser annealing as a means to locally tune the optical resonance of Er 3+ emitters in TiO 2 thin films on Si. Using both nanoscale x-ray diffraction measurements and cryogenic photoluminescence spectroscopy, we show that tightly focused below-gap laser annealing can induce anatase to rutile phase transitions in a nearly diffraction-limited area of the films and improve local crystallinity through grain growth. As a percentage of Er:TiO 2 is converted to rutile, the Er 3+ optical transition blueshifts by 13 nm. We explore the effects of changing laser annealing time and show that the amount of optically active Er:rutile increases linearly with laser power. We additionally demonstrate local phase conversion on microfabricated Si structures, which holds significance for quantum photonics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Exploring transport-enabled gates with integrated optical addressing to demonstrate high fidelity control of trapped ion qubits in a scalable quantum computer

In recent years, experiments involving micofabricated surface ion traps have grown in complexity, and as this complexity grows, a common design has emerged in the form of quantum charge-coupled device architecture. This architecture, already utilized on multiple systems, supports multiple zones on a device for areas such as memory or computation. The shutting process between these zones is a process often seen to be minimized. An additional component to scalable surface trapped-ion experiments includes some form of integrated photonics, as free space lasers have difficulty scaling to many ions. Here, we discuss recent results in utilizing the shuttling process with integrated photonics to perform a specific type of gate, as well as demonstrating state preparation. Furthermore, we show that these gates can be utilized as a type of optical modulator as the Doppler shift that occurs during shuttling will make the light seen by shuttled ions different than that seen by stationary ions. Furthermore, we show that the shuttling operation can be utilized as an optical modulator, where the Doppler shift changes the frequency from that of a stationary ion.

42 ENGINEERING↗
DOE OSTI2021

Optical coherence and energy-level properties of a Tm 3+ -doped LiNbO 3 waveguide at subKelvin temperatures

We characterize the optical coherence and energy-level properties of the 795-nm 3 H 6 to 3 H 4 transition of Tm 3+ in a Ti 4+ :LiNbO 3 waveguide at temperatures as low as 0.65 K. Coherence properties are measured with varied temperature, magnetic field, optical excitation power and wavelength, and measurement timescale. We also investigate nuclear spin-induced hyperfine structure and population dynamics with varying magnetic field and laser excitation power. Except for accountable differences due to different Ti 4+ - and Tm 3+ -doping concentrations, we find that the properties of Tm 3+ :Ti 4+ :LiNbO 3 produced by indiffusion doping are consistent with those of a bulk-doped Tm 3+ :LiNbO 3 crystal measured under similar conditions. Furthermore, our results, which complement previous work in a narrower parameter space, support using rare-earth ions for integrated optical and quantum signal processing.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2025

Vibrational Signatures of Electronic Properties in Renewable-Energy Catalysis

The objective of this research program is to discover and develop new approaches for ab initio computational simulations of molecular motion. Specifically, this program aims to decipher the connection between the underlying electronic structure and the accordant molecular vibrations in reactive ions and radicals for renewable-energy purposes. Recent experimental progress in ion sources and optical spectroscopies has unearthed considerable new inner-sphere detail for these complexes, but the connection between these spectral signatures and mechanistic information often remains elusive, to the continued frustration of experimentalists. For this purpose, new anharmonic vibrational frequency methods, along with a publicly deployed software package, will be developed. Working closely with committed experimental collaborators, this conceptual and computational framework will be used to explain the results of new spectroscopy experiments, focusing specifically on the inner-shell mechanisms of renewable-energy catalysis. The oxidation half of catalytic water-splitting chemistry will be a central focus, along with fundamental studies of the manner in which strong ions and radicals activate solvent as a chemical species. The resulting products of the research program will include openly available software and algorithms for the ab initio simulation of challenging vibrational spectra, as well as critical mechanistic insight into energy-focused catalytic processes that are opaque to other existing analytical techniques.

42 ENGINEERING↗
DOE OSTI2020

Dipole-Phonon Quantum Logic with Trapped Polar Molecular Ions

The interaction between the electric dipole moment of a trapped molecular ion and the phonon modes of the confined Coulomb crystal couples the orientation of the molecule to its motion. We consider the practical feasibility of harnessing this interaction to initialize, process, and read out quantum information encoded in molecular ion qubits without ever optically illuminating the molecules. We present two schemes wherein a molecular ion can be entangled with a cotrapped atomic ion qubit, providing, among other things, a means for molecular state preparation and measurement. Here, we also show that virtual phonon exchange can significantly boost the range of the intermolecular dipole-dipole interaction, allowing strong coupling between widely separated molecular ion qubits.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Optical Microscopy-Guided Laser Ablation Electrospray Ionization Ion Mobility Mass Spectrometry: Ambient Single Cell Metabolomics with Increased Confidence in Molecular Identification

Single cell analysis is a field of increasing interest as new tools are continually being developed to understand intercellular differences within large cell populations. Laser-ablation electrospray ionization mass spectrometry (LAESI-MS) is an emerging technique for single cell metabolomics. Over the years, it has been validated that this ionization technique is advantageous for probing the molecular content of individual cells in situ. Here, we report the integration of a microscope into the optical train of the LAESI source to allow for visually informed ambient in situ single cell analysis. Additionally, we have coupled this ‘LAESI microscope’ to a drift-tube ion mobility mass spectrometer to enable separation of isobaric species and allow for the determination of ion collision cross sections in conjunction with accurate mass measurements. This combined information helps provide higher confidence for structural assignment of molecules ablated from single cells. Here, we show that this system enables the analysis of the metabolite content of Allium cepa epidermal cells with high confidence structural identification together with their spatial locations within a tissue.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

The persistence of memory in ionic conduction probed by nonlinear optics

Predicting practical rates of transport in condensed phases enables the rational design of materials, devices and processes. This is especially critical to developing low-carbon energy technologies such as rechargeable batteries. For ionic conduction, the collective mechanisms, variation of conductivity with timescales and confinement, and ambiguity in the phononic origin of translation, call for a direct probe of the fundamental steps of ionic diffusion: ion hops. However, such hops are rare-event large-amplitude translations, and are challenging to excite and detect. Here we use single-cycle terahertz pumps to impulsively trigger ionic hopping in battery solid electrolytes. This is visualized by an induced transient birefringence, enabling direct probing of anisotropy in ionic hopping on the picosecond timescale. The relaxation of the transient signal measures the decay of orientational memory, and the production of entropy in diffusion. We extend experimental results using in silico transient birefringence to identify vibrational attempt frequencies for ion hopping. Using nonlinear optical methods, we probe ion transport at its fastest limit, distinguish correlated conduction mechanisms from a true random walk at the atomic scale, and demonstrate the connection between activated transport and the thermodynamics of information.

25 ENERGY STORAGE↗
DOE OSTI2022

Alkaline-Earth Chalcogenide Nanocrystals: Solution-Phase Synthesis, Surface Chemistry, and Stability

Increasing demand for effective energy conversion materials and devices has renewed interest in semiconductors comprised of earth-abundant and biocompatible elements. Alkaline-earth sulfides doped with rare earth ions are versatile optical materials. However, relatively little is known about controlling the dimensionality, surface chemistry, and inherent optical properties of the undoped versions of alkaline-earth monoand polychalcogenides. Here, we describe the colloidal synthesis of alkaline-earth chalcogenide nanocrystals through the reaction of metal carboxylates with carbon disulfide or selenourea. Systematic exploration of the synthetic phase space allows us to tune particle sizes over a wide range using a mixture of commercially available carboxylate precursors. Solid-state NMR spectroscopy confirms the phase purity of the selenide compositions. Surface characterization reveals that bridging carboxylates and amines preferentially terminate the surface of the nanocrystals. While these materials are colloidally stable in the mother solution, the selenides are susceptible to oxidation over time, eventually degrading to selenium metal through polyselenide intermediates. As part of these investigations, we have developed the colloidal syntheses of barium di- and triselenides, two among few reported nanocrystalline alkaline-earth polychalcogenides. Electronic structure calculations reveal that both materials are indirect band gap semiconductors. The colloidal chemistry presented here may enable the synthesis of more complex, multinary chalcogenide materials containing alkaline-earth elements.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Quantum computing universal thermalization dynamics in a (2 + 1)D Lattice Gauge Theory

Simulating non-equilibrium phenomena in strongly-interacting quantum many-body systems, including thermalization, is a promising application of near-term and future quantum computation. By performing experiments on a digital quantum computer consisting of fully-connected optically-controlled trapped ions, we study the role of entanglement in the thermalization dynamics of a Z 2 lattice gauge theory in 2+1 spacetime dimensions. Using randomized-measurement protocols, we efficiently learn a classical approximation of non-equilibrium states that yields the gap-ratio distribution and the spectral form factor of the entanglement Hamiltonian. These observables exhibit universal early-time signals for quantum chaos, a prerequisite for thermalization. Our work, therefore, establishes quantum computers as robust tools for studying universal features of thermalization in complex many-body systems, including in gauge theories.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2023

Quantum simulation of conical intersections using trapped ions

Conical intersections often control the reaction products of photochemical processes and occur when two electronic potential energy surfaces intersect. Theory predicts that the conical intersection will result in a geometric phase for a wavepacket on the ground potential energy surface, and although conical intersections have been observed experimentally, the geometric phase has not been directly observed in a molecular system. Herein we use a trapped atomic ion system to perform a quantum simulation of a conical intersection. The ion’s internal state serves as the electronic state, and the motion of the atomic nuclei is encoded into the motion of the ions. The simulated electronic potential is constructed by applying state-dependent optical forces to the ion. We experimentally observe a clear manifestation of the geometric phase using adiabatic state preparation followed by motional state measurement. Our experiment shows the advantage of combining spin and motion degrees for quantum simulation of chemical reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

A portable fiber optic sensor for the luminescent sensing of cobalt ions using carbon dots

Cobalt is critical to energy-relevant technologies, and demand for cobalt will increase significantly with growing global adoption of renewables. However, supply chain stability is threatened by economic and geopolitical factors, incentivizing domestic cobalt production from alternative resources such as coal, coal utilization byproducts (e.g., ash, acid mine drainage) and electronic waste. Rapid, inexpensive, and portable characterization techniques are needed to reduce production costs associated with cobalt prospecting and process monitoring. Here, in this research, we develop a compact, portable fiber optic luminescent probe for cobalt using phosphorus and nitrogen co-doped carbon dots as the sensing material. The carbon dot emission overlaps well with the cobalt absorption band at ~510 nm, leading to a selective decrease in emission as a function of cobalt concentration. The system responds nearly instantly to the presence of cobalt, with detection limits of 0.7 and 3.5 ppm in water and pH 1.68 buffer, respectively, providing comparable performance to a commercial spectrometer at a significantly lower cost. Moreover, the sensor is selective for cobalt in the presence of 13 of the most common metal ions encountered in coal utilization byproducts and is responsive to cobalt when spiked into an acid mine drainage leachate sample, highlighting the sensor's potential for real-world deployment in challenging matrices. In addition, integrating the carbon dots with a filter paper substrate produced ‘test strip’ sensors that exhibited a selective and sensitive visual response to cobalt using a handheld UV lamp. Taken together, the sensing system represents a significant step forward in the development of low-cost practical sensors for high-value metals in complex streams.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗