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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 217 records · Page 12
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

High-precision chemical quantum sensing in flowing monodisperse microdroplets

A method is presented for high-precision chemical detection that integrates quantum sensing with droplet microfluidics. Using nanodiamonds (ND) with fluorescent nitrogen-vacancy (NV) centers as quantum sensors, rapidly flowing microdroplets containing analyte molecules are analyzed. A noise-suppressed mode of optically detected magnetic resonance is enabled by pairing controllable flow with microwave control of NV electronic spins, to detect analyte-induced signals of a few hundredths of a percent of the ND fluorescence. Using this method, paramagnetic ions in droplets are detected with low limit-of-detection using small analyte volumes, with exceptional measurement stability over >10 3 s. In addition, these droplets are used as microconfinement chambers by co-encapsulating ND quantum sensors with various analytes such as single cells, suggesting wide-ranging applications including single-cell metabolomics and real-time intracellular measurements from bioreactors. Important advances are enabled by this work, including portable chemical testing devices, amplification-free chemical assays, and chemical imaging tools for probing reactions within microenvironments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Biophotonic rogue waves in red blood cell suspensions

Rogue waves are ubiquitous in nature, appearing in a variety of physical systems ranging from acoustics, microwave cavities, optical fibers, and resonators to plasmas, superfluids, and Bose–Einstein condensates. Unlike nonlinear solitary waves, rogue waves are extreme events that can occur even without nonlinearity by, for example, spontaneous synchronization of waves with different spatial frequencies in a linear system. Here, we report the observation of rogue-wave-like events in human red blood cell (RBC) suspensions under weak light illumination, characterized by an abnormal L-shaped probability distribution. Such biophotonic extreme events arise mostly due to the constructive interference of Mie-scattered waves from the suspended RBCs, whose biconcave shape and mutable orientation give rise to a time-dependent random phase modulation to an incident laser beam. We numerically simulate the beam propagation through the colloidal suspensions with added disorder in both spatial and temporal domains to mimic random scattering due to Brownian motion. In addition, at high power levels, nonlinear beam self-focusing is also observed, leading to a dual-exponential probability distribution associated with the formation of multiple soliton-like spots. Such rogue wave events should also exist in environments with cells of other species such as swimming bacteria, and understanding of their underlying physics may lead to unexpected biophotonic applications.

59 BASIC BIOLOGICAL SCIENCES↗
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 OSTI2025

Nitrogen Vacancy Center in Diamond for the Stress and Field Sensing Applications

The nitrogen-vacancy (NV) center in a nanodiamond (ND) crystal is a promising material for quantum information processing, sensing, and computing applications. It is one of the best candidate materials for quantum sensing and metrology expected to work at elevated temperatures and pressures conditions. We computationally show the effect of strain on the defect band edges and band gaps in the NV center diamond. A low energy Hamiltonian is developed for the ±1 spin manifold at the ground state. We show the quantum sensing device is a few orders of magnitude superior in sensing than the traditional optical sensing devices. We also discuss experimental results from the optically detected magnetic resonance (ODMR) and the spin relaxometry for the field sensing applications. The presentation concludes by providing a model for free spins detection of the rare earth ions.

field sensing applications↗
DOE OSTI2025

Synthesis of nanodiamonds encapsulated by zeolitic imidazole framework-8 for quantum sensing applications

Nitrogen vacancy (NV)-containing nanodiamonds are widely used in quantum sensing applications due to their high sensitivity to magnetic fields, relatively low cost, and ability to be initialized, manipulated, and read out at room temperature. Quantum sensing techniques such as optically detected magnetic resonance (ODMR) and spin relaxometry have exploited the sensitivity of the NV nanodiamonds to magnetic fields to detect a range of analytes, such as pH, metal ions, and biomolecules. However, diversifying the sensing targets accessible by NV diamond quantum sensors typically requires careful engineering of the diamond surface chemistry with stimuli-responsive functional groups. Here, a simple protocol for coating NV nanodiamonds with the zeolitic imidazole framework 8 (ZIF-8), a widely used metal-organic framework, is presented. ZIF-8 is a highly porous material that has been used as a selective sensor for gasses, metal ions, and other analytes. The material is well-characterized by x-ray diffraction, transmission electron microscopy, scanning electron microscopy, x-ray photoelectron spectroscopy, and luminescence spectroscopy. Encapsulation of NV nanodiamonds with a porous scaffold such as ZIF-8 provides a promising method for improving the selectivity for the quantum sensing of various analytes. Importantly, the ZIF-8 coating does not impact the luminescence properties of the NV diamond, which is a key readout in ODMR and spin relaxometry sensing approaches. Indeed, the ODMR spectra with and without the ZIF-8 shell is nearly identical. Moreover, the ZIF-8 coating increases the longitudinal spin relaxation time of the NV nanodiamond by a factor of 4 relative to aggregated diamond, a desirable outcome for spin relaxation-based quantum sensing. Metal-organic framework composites with nanodiamonds thus are an exciting strategy for enhancing NV nanodiamond performance in applications such as quantum sensing and quantum-enhanced nuclear magnetic resonance spectroscopy.

nitrogen vacancy nanodiamond↗
DOE OSTI2021

Neutron Radiography and Computed Tomography of Biological Systems at the Oak Ridge National Laboratory's High Flux Isotope Reactor

Neutrons have historically been used for a broad range of biological applications employing techniques such as small-angle neutron scattering, neutron spin echo, diffraction, and inelastic scattering. Unlike neutron scattering techniques that obtain information in reciprocal space, attenuation-based neutron imaging measures a signal in real space that is resolved on the order of tens of micrometers. The principle of neutron imaging follows the Beer-Lambert law and is based on the measurement of the bulk neutron attenuation through a sample. Greater attenuation is exhibited by some light elements (most notably, hydrogen), which are major components of biological samples. Contrast agents such as deuterium, gadolinium, or lithium compounds can be used to enhance contrast in a similar fashion as it is done in medical imaging, including techniques such as optical imaging, magnetic resonance imaging, X-ray, and positron emission tomography. For biological systems, neutron radiography and computed tomography have increasingly been used to investigate the complexity of the underground plant root network, its interaction with soils, and the dynamics of water flux in situ. Moreover, efforts to understand contrast details in animal samples, such as soft tissues and bones, have been explored. This manuscript focuses on the advances in neutron bioimaging such as sample preparation, instrumentation, data acquisition strategy, and data analysis using the High Flux Isotope Reactor CG-1D neutron imaging beamline. The aforementioned capabilities will be illustrated using a selection of examples in plant physiology (herbaceous plant/root/soil system) and biomedical applications (rat femur and mouse lung).

Bilheux, Hassina↗
DOE OSTI2024

Overview of Quantum Sensing Materials and Techniques for Energy Sector Applications

The energy sector has become increasingly dependent upon highly sensitive sensing devices for a wide range of applications. Variables such as temperature, pH, electromagnetic fields, ions, and pressure must be measured with high precision, often in harsh conditions (e.g. highly corrosive environments due to 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, and critical mineral deposits. The continued maturation of quantum sensing technologies offers exciting opportunities for quantum-enhanced measurements within the energy sector that may provide significant improvements in sensitivity beyond the classical limit. Here, an overview of established and emerging quantum materials for sensing applications will be provided, from trapped ions to color centers in diamond and silicon carbide. Associated quantum sensing methods for these materials will be discussed, with an emphasis on platforms that are nearing commercial viability. Specific application 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 measurement in electric vehicle batteries, and quantum-enhanced spectroscopy. Remaining barriers, such as quantum sensor platform miniaturization and ruggedization, will also be analyzed. A specific project at the National Energy Technology Laboratory involving the functionalization of qubits using metal-organic frameworks for enhanced quantum sensing will also 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 in a controlled way using the metal-organic framework ZIF-8. The ZIF-8 provides a well-defined, porous scaffold that can be controlled to promote the selective uptake of specific target analytes, such as gas molecules or ions. The quantum sensing performance of this composite material is either preserved or enhanced following ZIF-8 encapsulation; the optically detected magnetic resonance response of the NV nanodiamonds with and without the ZIF-8 coating are identical, while the ZIF-8 coating increases the longitudinal spin relaxation lifetime (T1) of the NV centers, an important parameter for spin relaxometry-based quantum sensing experiments. Taken together, these results demonstrate the importance of qubit functionalization as a crucial step for rationally designing high performance quantum sensors.

Crawford, Scott↗
DOE OSTI2021

Integrated reference cavity with dual-mode optical thermometry for frequency correction

Photonic integrated resonators have advantages over traditional benchtop cavities in terms of size, weight, and cost with the potential to enable applications that require spectrally pure light. However, integrated resonators suffer from temperature-dependent frequency variations and are sensitive to external environmental perturbations, which hinders their usage in precision frequency applications. One solution is to use interrogation of the cavity temperature through dual-mode optical thermometry (DMOT) by measuring the shift of the resonance frequency difference between two polarization or optical frequency modes. Yet this approach has only been demonstrated in bulk-optic whispering gallery mode and fiber resonators. In this paper, we implement dual-mode optical thermometry in an ultra-high Q integrated silicon nitride resonator. A dual-mode resonance frequency difference temperature sensitivity of 188 ± <#comment/> 15 M H z / K is measured. We demonstrate feedforward DMOT frequency correction that, under an applied external temperature ramp, is able to reduce the optical frequency change to 0.31 kHz/s as compared to an uncorrected 10.03 kHz/s, a factor of 30 × <#comment/> reduction. These results show promise for on-chip frequency correction solutions for quantum, metrology, atomic, and coherent optical communications applications.

Zhao, Qiancheng (ORCID:0000000206968667)↗
DOE OSTI2022

Optical Response of Periodic Arrays of Graphene Nanodisks

Doped graphene nanostructures are a promising platform for photonics due to their exceptionally strong and tunable plasmonic resonances. When placed in a periodic array configuration, the plasmons supported by the individual nanostructures interact with each other and, under the appropriate conditions, can give rise to a collective mode known as a lattice resonance. Here, for this study, we perform a comprehensive analysis of the response of periodic arrays of graphene nanodisks and identify the conditions under which the system is able to support lattice resonances. We find that the ratio between the period of the array and the wavelength of the plasmon completely determines the behavior of the system. As a consequence, strong lattice resonances are achieved for micron-size nanodisks in the terahertz regime. We develop a theoretical model valid beyond the electrostatic approximation and use it to derive closed analytical expressions for the strength, the wavelength, and the width of the optical resonance of the arrays. The theoretical framework developed in this work paves the way for facile design and discovery of emerging properties of periodic arrays of graphene nanostructures that could enable applications in photonics and plasmonics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

ac Sensing Using Nitrogen-Vacancy Centers in a Diamond Anvil Cell up to 6 GPa

Nitrogen-vacancy color centers in diamond have attracted broad attention as quantum sensors for both static and dynamic magnetic, electrical, strain, and thermal fields and are particularly attractive for quantum sensing under pressure in diamond anvil cells. Optically based nuclear magnetic resonance may be possible at pressures greater than a few gigapascals and offers an attractive alternative to conventional Faraday-induction-based detection. In this work, we present ac sensing results and demonstrate synchronized readout up to 6 GPa but find that the sensitivity is reduced due to inhomogeneities of the microwave field and pressure within the sample space. These experiments enable the possibility of all-optical high resolution magnetic resonance of nanoliter sample volumes at high pressures.

58 GEOSCIENCES↗
DOE OSTI2023

Nanophotonic quantum sensing with engineered spin-optic coupling

Nitrogen vacancy centers in diamond provide a spin-based qubit system with long coherence time even at room temperature, making them suitable ambient-condition quantum sensors for quantities including electromagnetic fields, temperature, and rotation. The optically addressable level structures of NV spins allow transduction of spin information onto light-field intensity. The sub-optimal readout fidelity of conventional fluorescence measurement remains a significant drawback for room-temperature ensemble sensing. Here, we discuss nanophotonic interfaces that provide opportunities to achieve near-unity readout fidelity based on IR absorption via resonantly enhanced spin-optic coupling. Spin-coupled resonant nanophotonic devices are projected to particularly benefit applications that utilize micro- to nanoscale sensing volume and to outperform present methods in their volume-normalized sensitivity.

42 ENGINEERING↗
DOE OSTI2020

Different Kinetic Reactivities of Electrons in Distinct TiO 2 Nanoparticle Trap States

Electrons added to TiO 2 and other semiconductors often occupy trap states, whose reactivity can determine the catalytic and stoichiometric chemistry of the material. We previously showed that reduced aqueous colloidal TiO 2 nanoparticles have two distinct classes of thermally equilibrated trapped electrons, termed Red/e – and Blue/e – . Presented here are parallel optical and electron paramagnetic resonance (EPR) kinetic studies of the reactivity of these electrons with solution-based oxidants. Optical stopped-flow measurements monitoring the reactions of TiO 2 /e – with substoichiometric oxidants showed a surprising pattern: an initial fast (seconds) decrease in TiO 2 /e – absorbance followed by a secondary, slow (minutes) increase in the broad TiO 2 /e – optical feature. The analysis revealed that the fast decrease is due to the preferential oxidation of the Red/e – trap states and the slow increase results from the re-equilibration of electrons from Blue/e - to Red/e - states. This kinetic model was confirmed by freeze-quench EPR measurements. Quantitative analysis of the kinetic data demonstrated that Red/e – react ~5 times faster than Blue/e – with the nitroxyl radical oxidant 4-methoxy-2,2,6,6-tetramethyl-1-piperidinyloxyl (4-MeO-TEMPO). Similar reactivity patterns were also observed in oxidations of TiO 2 /e – by O 2 , which like 4-MeO-TEMPO is a proton-coupled electron transfer (PCET) oxidant, and by the pure electron transfer (ET) oxidant potassium triiodide (KI 3 ). Furthermore, this suggests that the faster intrinsic reactivity of one trap state over another on the seconds–minutes time scale is likely a general feature of reduced TiO 2 reactivity. This differential trap-state reactivity is likely to influence the performance of TiO 2 in photochemical/electrochemical devices, and it suggests an opportunity for tuning catalysis.

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

Long-range cooperative resonances in rare-earth ion arrays inside photonic resonators

Engineering arrays of active optical centers to control the interaction Hamiltonian between light and matter has been the subject of intense research recently. Collective interaction of atomic arrays with optical photons can give rise to directionally enhanced absorption or emission, which enables engineering of broadband and strong atom-photon interfaces. Here, we report on the observation of long-range cooperative resonances in an array of rare-earth ions controllably implanted into a solid-state lithium niobate micro-ring resonator. We show that cooperative effects can be observed in an ordered ion array extended far beyond the light’s wavelength. We observe enhanced emission from both cavity-induced Purcell enhancement and array-induced collective resonances at cryogenic temperatures. Engineering collective resonances as a paradigm for enhanced light-matter interactions can enable suppression of free-space spontaneous emission. The multi-functionality of lithium niobate hosting rare-earth ions can open possibilities of quantum photonic device engineering for scalable and multiplexed quantum networks.

42 ENGINEERING↗
DOE OSTI2021

Multimodal Tip-Enhanced Nonlinear Optical Nanoimaging of Plasmonic Silver Nanocubes

Optical field localization at plasmonic tip-sample nanojunctions has enabled high spatial resolution chemical analysis through tip-enhanced linear optical spectroscopies, including Raman scattering and photoluminescence. In this work, we illustrate that nonlinear optical processes, including parametric four-wave mixing (4WM), second harmonic/sum-frequency generation (SHG and SFG), and two-photon photoluminescence (TPPL), can be enhanced at plasmonic junctions and spatio-spectrally resolved simultaneously with few-nm spatial resolution under ambient conditions. More importantly, through a detailed analysis of our spectral nano-images, we find that the efficiencies of the local nonlinear signals are determined by sharp tip-sample junction resonances that vary over the few-nanometer length scale because of the corrugated nature of the probe. Namely, plasmon resonances centered at or around the different nonlinear signals are tracked through TPPL, and they are found to selectively enhance nonlinear signals with closely matched optical resonances.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Near field excited state imaging via stimulated electron energy gain spectroscopy of localized surface plasmon resonances in plasmonic nanorod antennas

Continuous wave (cw) photon stimulated electron energy loss and gain spectroscopy (sEELS and sEEGS) is used to image the near field of optically stimulated localized surface plasmon resonance (LSPR) modes in nanorod antennas. An optical delivery system equipped with a nanomanipulator and a fiber-coupled laser diode is used to simultaneously irradiate plasmonic nanostructures in a (scanning) transmission electron microscope. The nanorod length is varied such that the m = 1, 2, and 3 LSPR modes are resonant with the laser energy and the optically stimulated near field spectra and images of these modes are measured. Various nanorod orientations are also investigated to explore retardation effects. Optical and electron beam simulations are used to rationalize the observed patterns. As expected, the odd modes are optically bright and result in observed sEEG responses. The m = 2 dark mode does not produce a sEEG response, however, when tilted such that retardation effects are operative, the sEEG signal emerges. Thus, we demonstrate that cw sEEGS is an effective tool in imaging the near field of the full set of nanorod plasmon modes of either parity.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Generalised hyper-Ramsey spectroscopy of two-level atoms in an optically dense medium

The peculiarities of Ramsey resonance and its sensitivity to the light shift from an optically dense medium of cold atoms are investigated. Different composite pulse protocols for clock spectroscopy, including hyper-Ramsey, modified and generalised hyper-Ramsey schemes, are compared. Error signals change significantly due to the processes of absorption and dispersion in the atomic medium. The dependence of the position of the central fringe resonance with a residual uncompensated light shift of the atomic transition is studied with the attenuation of the radiation intensity in the medium taken into account. It is shown that using a combination of generalised hyper-Ramsey error signals allows one to suppress the sensitivity to the light shift for any length of the medium. (laser cooling of atoms)

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Optical readout of singlet fission biexcitons in a heteroacene with photoluminescence detected magnetic resonance

Molecular spin systems based on photoexcited triplet pairs formed via singlet fission (SF) are attractive as carriers of quantum information because of their potentially pure and controllable spin polarization, but developing systems that offer optical routes to readout as well as initialization is challenging. Herein, we characterize the electron spin magnetic resonance change in the photoluminescence intensity for a tailored organic molecular crystal while sweeping a microwave drive up to 10 GHz in a broadband loop structure. We observe resonant transitions for both triplet and quintet spin sublevel populations showing their optical sensitivity and revealing the zero-field parameters for each. We map the evolution of these spectra in both microwave frequency and magnetic field, producing a pattern of optically detected magnetic resonance (ODMR) peaks. Fits to these data using a suitable model suggest significant spin polarization in this system with orientation selectivity. Unusual excitation intensity dependence is also observed, which inverts the sign of the ODMR signal for the triplet features, but not for the quintet. These observations demonstrate optical detection of the spin sublevel population dictated by SF and intermolecular geometry, and highlight anisotropic and multi-scale dynamics of triplet pairs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗