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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 55 records · Page 3
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

A Time-Gated, Time-Correlated Single-Photon-Counting Lidar to Observe Atmospheric Clouds at Submeter Resolution

Most lidars used for cloud observations have the range resolution of about 10 m, so they are incapable of resolving submeter-scale processes that are crucial to cloud evolution. This article describes a prototype of a ground-based, vertically pointing, time-gated, time-correlated single-photon-counting lidar (referred to as the T2 lidar) developed to explore atmospheric clouds at range resolution two orders of magnitude finer than traditional atmospheric lidars. The T2 lidar emits green-light pulses (532 nm) at a repetition rate of 20.6 kHz and a pulse width of ∼650 ps, which enables the observation of aerosol and cloud layers at heights from a few hundred meters to 7.28 km above the ground level at range resolution down to 10 cm. In addition, a digital delay pulse generator controls the detector to only receive photons for a short period after each laser pulse. This time-gated technique blocks photons arriving from regions outside the target zone, thus significantly reducing the noise level and allowing observation even inside clouds. Initial observations show that the T2 lidar can detect sharp cloud boundaries and fine structures near the cloud base. Such refined measurements of cloud structure could lead to an improved understanding of microphysical processes such as droplet activation, entrainment and mixing, and precipitation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

HERMES

HERMES - High-speed Event Retrieval and Management for Enhanced Spectral imaging code. This code is meant to unpack and process neutron imaging data from the TPX3Cam made by Amsterdam Scientific Instruments. The TPX3Cam utilizes the Timepix3 chip in a single photon counting mode of image acquisition. The photon counting data streaming off the TPX3Cam needs to be process and analyzed in order to create final images. Therefore we are developing both python and cpp codes to allow for users of the TPX3Cam to efficiently analyze data and create images.

Long, Alexander↗
DOE OSTI2024

Measuring Intermolecular Excited State Geometry for Favorable Singlet Fission in Tetracene

Singlet fission (SF) is the process of converting an excited singlet to a pair of excited triplets. Harvesting two charges from a single photon has the potential to increase photovoltaic device efficiencies. Acenes, such as tetracene and pentacene, are model molecules for studying SF. Despite SF being an endoergic process for tetracene and exoergic for pentacene, both acenes exhibit near unity SF quantum efficiencies, raising questions about how tetracene can overcome the energy barrier. Here, we use recently developed instrumentation to measure inelastic neutron scattering (INS) while optically exciting the model molecules using two different excitation energies. The spectroscopic results reveal intermolecular structural relaxation due to the presence of a triplet excited state. Here, the structural dynamics of the combined excited state molecule and surrounding tetracene molecules are further studied using time-dependent density functional theory (TD-DFT), which shows that the singlet and triplet levels shift due to the excited state geometry, reducing the uphill energy barrier for SF to within kT.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Spectral control of nonclassical light pulses using an integrated thin-film lithium niobate modulator

Abstract Manipulating the frequency and bandwidth of nonclassical light is essential for implementing frequency-encoded/multiplexed quantum computation, communication, and networking protocols, and for bridging spectral mismatch among various quantum systems. However, quantum spectral control requires a strong nonlinearity mediated by light, microwave, or acoustics, which is challenging to realize with high efficiency, low noise, and on an integrated chip. Here, we demonstrate both frequency shifting and bandwidth compression of heralded single-photon pulses using an integrated thin-film lithium niobate (TFLN) phase modulator. We achieve record-high electro-optic frequency shearing of telecom single photons over terahertz range (±641 GHz or ±5.2 nm), enabling high visibility quantum interference between frequency-nondegenerate photon pairs. We further operate the modulator as a time lens and demonstrate over eighteen-fold (6.55 nm to 0.35 nm) bandwidth compression of single photons. Our results showcase the viability and promise of on-chip quantum spectral control for scalable photonic quantum information processing.

Optics↗
DOE OSTI2021

Leveraging lifetime information to perform real-time 3D single-particle tracking in noisy environments

A microscopy platform that leverages the arrival time of individual photons to enable 3D single-particle tracking of fast-moving (translational diffusion coefficient of ≃ 3.3 µm 2 /s) particles in high-background environments is reported here. It combines a hardware-based time-gating module, which enables the rate of photon processing to be as high as 100 MHz, with a two-photon excited 3D single-particle tracking confocal microscope to enable high sample penetration depth. Proof-of-principle experiments where single quantum dots are tracked in solutions containing dye-stained cellulose are shown, with tracking performance markedly improved using the hardware-based time-gating module. Furthermore, such a microscope design is anticipated to be of use to a variety of communities who wish to track single-particles in cellular environments, which commonly have high fluorescence and scattering background.

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

Hidden domain boundary dynamics toward crystalline perfection

A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies. Here, we apply ultrafast single-shot X-ray photon correlation spectroscopy to resolve the nonequilibrium, heterogeneous, and irreversible mesoscale dynamics during a light-induced phase transition in a (PbTiO 3 ) 16 /(SrTiO 3 ) 16 superlattice. Such ferroelectric superlattice systems are a useful platform to study phase transitions and topological dynamics due to their high degree of tunability. This provides an approach for capturing the nucleation of the light-induced phase, the formation of transient mesoscale defects at the boundaries of the nuclei, and the eventual annihilation of these defects, even in systems with complex polarization topologies. We identify a nonequilibrium correlation response spanning >10 orders of magnitude in timescales, with multistep behavior similar to the plateaus observed in supercooled liquids and glasses. We further show how the observed time-dependent long-time correlations can be understood in terms of stochastic and non-Markovian dynamics of domain walls, encoded in waiting-time distributions with power-law tails. This work defines possibilities for probing the nonequilibrium and correlated dynamics of disordered and heterogeneous media.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Single-photon detection using high-temperature cuprate superconductors

The detection of individual quanta of light is important for quantum computation, fluorescence lifetime imaging, single-molecule detection, remote sensing, correlation spectroscopy, and more. Thanks to their broadband operation, high detection efficiency, exceptional signal-to-noise ratio, and fast recovery times, superconducting nanowire single-photon detectors (SNSPDs) have become a critical component in these applications. The operation of SNSPDs based on conventional superconductors, which have a low critical temperature (T c ), requires costly and bulky cryocoolers. This motivated exploration of other superconducting materials with higher T c that would enable single-photon detection at elevated temperatures, yet this task has proven exceedingly difficult. Here we show that with proper processing, high-T c cuprate superconductors can meet this challenge. We fabricated superconducting nanowires (SNWs) out of thin flakes of Bi 2 Sr 2 CaCu2O 8+δ and La 1.55 Sr 0.45 CuO 4 /La 2 CuO 4 (LSCO-LCO) bilayer films and demonstrated their single-photon response up to 25 and 8 K, respectively. The single-photon operation is revealed through the linear scaling of the photon count rate (PCR) on the radiation power. Both of our cuprate-based SNSPDs exhibited single-photon sensitivity at the technologically-important 1.5 μm telecommunications wavelength. Our work expands the family of superconducting materials for SNSPD technology, opens the prospects of raising the temperature ceiling, and raises important questions about the underlying mechanisms of single-photon detection by unconventional superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Three Photon Excited Image Scanning Microscopy for in-Depth Super-Resolution Studies of Biological Samples

Multiphoton laser scanning microscopy is a powerful tool for deep imaging of thick biological samples. Image scanning microscopy (ISM) has demonstrated significant improvements in the signal-to-noise ratio in confocal laser scanning microscopy, while at the same time improving upon the effectively attainable resolution. Two-photon excitation (2PE), combined with ISM, has been shown to allow for deep tissue imaging with enhanced resolution compared to 2PE microscopy. Three-photon excitation (3PE) has enabled record imaging depth and contrast for multiphoton imaging, due to the superior suppression of out-of-focus signal generation. In this paper, we demonstrate super-resolution 3PE ISM. This is achieved using a single-photon avalanche detector array, and 1040-nm pulses for 3PE of blue fluorescence. This method enables subdiffraction limited resolution imaging of biological samples stained with blue fluorescent markers, such as mouse myocardial and spinal cord tissues stained with 4 ′ , 6 -diamidino-2-phenylindole. Deconvolution improves the resolving power further and allows for imaging with better than λ / 8 resolution with respect to the 3PE wavelength λ . With the ISM pixel reassignment procedure, we demonstrate a resolution enhancement of ∼ 1.6 laterally, compared to the resolution attained using a photomultiplier tube in a non-descanned detection arrangement, and a factor of ∼ 1.8 enhancement in axial resolution. The experimentally measured three-dimensional point spread function volume is shrunk ∼ 4.4 -fold, which is close to the theoretically expected enhancement. Published by the American Physical Society 2024

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Photoreactive Carbon Dioxide Capture by a Zirconium–Nanographene Metal–Organic Framework

Here, the mechanism of photochemical CO 2 reduction to formate by PCN-136, a Zr-based metal-organic framework (MOF) that incorporates light-harvesting nanographene ligands, has been investigated using steady-state and time-resolved spectroscopy and density functional theory (DFT) calculations. The catalysis was found to proceed via a "photoreactive capture" mechanism, where Zr-based nodes serve to capture CO 2 in the form of Zr- bicarbonates, while the nanographene ligands have a dual role of absorbing light and storing one-electron equivalents for catalysis. We also find that the process occurs via a "two-for-one" route, where a single photon initiates a cascade of electron/hydrogen atom transfers from the sacrificial donor to the CO 2 -bound MOF. The mechanistic findings obtained here illustrate several advantages of MOF-based architectures in molecular photocatalyst engineering and provide insights on ways to achieve high formate selectivity.

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

Single photon emitters in van der Waals solids for quantum photonics: materials, theory and molecular-scale characterization probes

Strong light–matter interactions in two-dimensional layered materials (2D materials) have attracted the interest of researchers from interdisciplinary fields for more than a decade now. A unique phenomenon in some 2D materials is their large exciton binding energies (BEs), increasing the likelihood of exciton survival at room temperature. It is this large BE that mediates the intense light–matter interactions of many of the 2D materials, particularly in their monolayer limit, where the interplay of excitonic phenomena poses a wealth of opportunities for high-performance optoelectronics and quantum photonics. Within quantum photonics, quantum information science (QIS) is growing rapidly, where photons are a promising platform for information processing due to their low-noise properties, excellent modal control, and long-distance propagation. A central element for QIS applications is a single photon emitter (SPE) source, where an ideal on-demand SPE emits exactly one photon at a time into a given spatiotemporal mode. Recently, 2D materials have shown practical appeal for QIS which is directly driven from their unique layered crystalline structure. This structural attribute of 2D materials facilitates their integration with optical elements more easily than the SPEs in conventional three-dimensional solid state materials, such as diamond and SiC. In this review article, we will discuss recent advances made with 2D materials towards their use as quantum emitters, where the SPE emission properties maybe modulated deterministically. Here, the use of unique scanning tunneling microscopy tools for the in-situ generation and characterization of defects is presented, along with theoretical first-principles frameworks and machine learning approaches to model the structure-property relationship of exciton–defect interactions within the lattice towards SPEs. Given the rapid progress made in this area, the SPEs in 2D materials are emerging as promising sources of nonclassical light emitters, well-poised to advance quantum photonics in the future.

2D layered materials↗
DOE OSTI2023

From Inside Out: How the Buried Interface, Shell Defects, and Surface Chemistry Conspire to Determine Optical Performance in Nonblinking Giant Quantum Dots

“Giant” or core/thick‐shell quantum dots (gQDs) are an important class of solid‐state quantum emitter characterized by strongly suppressed blinking and photobleaching under ambient conditions, and reduced nonradiative Auger processes. Together, these qualities provide distinguishing and useful functionality as single‐ and ensemble‐photon sources. For many applications, operation at elevated temperatures and under intense photon flux is desired, but performance is strongly dependent on the synthetic method employed for thick‐shell growth. Here, a comprehensive analysis of gQD structural properties “from the inside out” as a function of shell‐growth method is reported: successive ionic layer adsorption and reaction (SILAR) and high‐temperature continuous injection (HT‐CI), or sequential combinations of the two. Key correlations across synthesis methods, structural features (interfacial alloying, stacking‐fault density and surface‐ligand identity), and performance metrics (quantum yield, single‐gQD photoluminescence under thermal/photo stress, charging behavior and quantum‐optical properties) are identified. Surprisingly, it is found that interfacial alloying is the strongest indicator of gQD stability under stress, but this parameter is not the determining factor for Auger suppression. Furthermore, quantum yield is strongly influenced by surface chemistry and can approach unity even in the case of high shell‐defect density, while introduction of zinc‐blende stacking faults increases the likelihood that a gQD exhibits charged‐state emission.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Systems for Transducing Entanglement Between Photons and Electron Spins

The transfer of quantum properties and entanglement between photons and matter (transduction) is a major challenge in QIS, especially with regard to networking quantum information processing. In order to overcome this challenge, it is important to know how non-classical light (single or entangled photons) interacts with matter. This project specifically addresses fundamental questions about the interaction of single and entangled photons with molecules and nanostructures to produce electrons with prescribed spin polarizations and pairs of electrons with entangled spins, thus resulting in transduction by addressing two major objectives: (2) In Objective 1, we will investigate the formation of polarization-encoded radical (spin qubit) pairs and molecular triplet states photoexcited by single quantum emitter light sources. (2) In Objective 2, we will demonstrate the use of two entangled photons, generated by spontaneous parametric down conversion (SPDC) or by the coherent biexcitonic states of perovskite NPLs, to produce two entangled radical (spin qubit) pairs or molecular triplet states.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

New Insights into Secondary Organic Aerosol Formation at the Air–Liquid Interface

Air-liquid interfacial processing of volatile organic compound oxidation has been suggested as an important source of secondary organic aerosols. However, owing to the lack of techniques for in situ air-liquid interface analysis, the detailed interfacial mechanism remains speculative. To obviate this, the analysis of air-liquid interfacial reactions and the dynamics of glyoxal oxidation as a model volatile organic compound using in situ liquid synchrotron-based vacuum ultraviolet single photon ionization mass spectrometry enabled by the system for analysis at the liquid vacuum interface microreactor is reported. This approach allows for determination of reaction intermediates and oxidation products including polymers and oligomers at the air-liquid interface by mass spectral analysis and appearance energy measurements. Furthermore, an expanded reaction mechanism of photooxidation free radical induced reactions as a source of aqueous secondary organic aerosol formation is proposed based on these new results, suggesting that single photon ionization could be applied to provide unique insights into interfacial chemistry changing the earth atmospheric composition.

aqueous secondary organic aerosol, glyoxal, photoo↗
DOE OSTI2023

The anisotropic nature of singlet fission in single crystalline organic semiconductors

The escalating global energy predicament implores for a revolutionary resolution—one that converts sunlight into electricity—holding the key to supreme conversion efficiency. This comprehensive review embarks on the exploration of the principle of generating multiple excitons per absorbed photon, a captivating concept that possesses the potential to redefine the fundamental confines of conversion efficiency, albeit its application remains limited in photovoltaic devices. At the nucleus of this phenomenon are two principal processes: multiple exciton generation (MEG) within quantum-confined environments, and singlet fission (SF) inside molecular crystals. The process of SF, characterized by the cleavage of a single photogenerated singlet exciton into two triplet excitons, holds promise to potentially amplify photon-to-electron conversion efficiency twofold, thereby laying the groundwork to challenge the detailed balance limit of solar cell efficiency. Our discourse primarily dissects the complex nature of SF in crystalline organic semiconductors, laying special emphasis on the anisotropic behavior of SF and the diffusion of the subsequent triplet excitons in single-crystalline polyacene organic semiconductors. We initiate this journey of discovery by elucidating the principles of MEG and SF, tracing their historical genesis, and scrutinizing the anisotropy of SF and the impact of quantum decoherence within the purview of functional mode electron transfer theory. We present an overview of prominent techniques deployed in investigating anisotropic SF in organic semiconductors, including femtosecond transient absorption microscopy and imaging as well as stimulated Raman scattering microscopies, and highlight recent breakthroughs linked with the anisotropic dimensions of Davydov splitting, Herzberg–Teller effects, SF, and triplet transport operations in single-crystalline polyacenes. Through this comprehensive analysis, our objective is to interweave the fundamental principles of anisotropic SF and triplet transport with the current frontiers of scientific discovery, providing inspiration and facilitating future ventures to harness the anisotropic attributes of organic semiconductor crystals in the design of pioneering photovoltaic and photonic devices.

Chemistry↗
DOE OSTI2020

Spectrally reconfigurable quantum emitters enabled by optimized fast modulation

The ability to shape photon emission facilitates strong photon-mediated interactions between disparate physical systems, thereby enabling applications in quantum information processing, simulation and communication. Spectral control in solid state platforms such as color centers, rare earth ions, and quantum dots is particularly attractive for realizing such applications on-chip. Here we propose the use of frequency-modulated optical transitions for spectral engineering of single photon emission. Using a scattering-matrix formalism, we find that a two-level system, when modulated faster than its optical lifetime, can be treated as a single-photon source with a widely reconfigurable photon spectrum that is amenable to standard numerical optimization techniques. To enable the experimental demonstration of this spectral control scheme, we investigate the Stark tuning properties of the silicon vacancy in silicon carbide, a color center with promise for optical quantum information processing technologies. We find that the silicon vacancy possesses excellent spectral stability and tuning characteristics, allowing us to probe its fast modulation regime, observe the theoretically-predicted two-photon correlations, and demonstrate spectral engineering. Our results suggest that frequency modulation is a powerful technique for the generation of new light states with unprecedented control over the spectral and temporal properties of single photons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Intersystem crossing and exciton–defect coupling of spin defects in hexagonal boron nitride

Despite the recognition of two-dimensional (2D) systems as emerging and scalable host materials of single-photon emitters or spin qubits, the uncontrolled, and undetermined chemical nature of these quantum defects has been a roadblock to further development. Leveraging the design of extrinsic defects can circumvent these persistent issues and provide an ultimate solution. Here, we established a complete theoretical framework to accurately and systematically design quantum defects in wide-bandgap 2D systems. With this approach, essential static and dynamical properties are equally considered for spin qubit discovery. In particular, many-body interactions such as defect–exciton couplings are vital for describing excited state properties of defects in ultrathin 2D systems. Meanwhile, nonradiative processes such as phonon-assisted decay and intersystem crossing rates require careful evaluation, which competes together with radiative processes. From a thorough screening of defects based on first-principles calculations, we identify promising single-photon emitters such as Si VV and spin qubits such as Ti VV and Mo VV in hexagonal boron nitride. This work provided a complete first-principles theoretical framework for defect design in 2D materials.

36 MATERIALS SCIENCE↗
DOE OSTI2026

High-Performance Near-Infrared Quantum Emission from Color Centers in hBN

Color centers hosted in hexagonal boron nitride (hBN) have emerged as a highly promising platform for single-photon emission and spin-photon technologies relevant to quantum communication and quantum networking. As a wide bandgap van der Waals material, hBN can host optically active quantum defects across a broad spectral range. Here, we demonstrate a simple and scalable oxygen-plasma process that reproducibly creates single quantum emitters in hBN with blinking-free zero-phonon lines (ZPLs) spanning near-infrared (NIR) from 700 up to 971 nm. These emitters combine MHz-level brightness, single-photon purity up to 99.9%, and ultranarrow cryogenic line widths down to 2.7 GHz under quasi-resonant excitation, placing them in a particularly attractive regime for quantum photonics. Photostability measurements further reveal resistance to photobleaching, subnanometer spectral stability over long time scales, and near-shot-noise-limited intensity fluctuations. Analysis of the phonon sidebands shows weak vibronic coupling and ZPL-dominated emission, with Debye–Waller factors approaching 50%. Control experiments together with elemental mapping support oxygen incorporation as a necessary ingredient in activating the NIR emitter population, while first-principles calculations identify O N V N and O N V N H as the leading defect candidates. These results establish a high-performance NIR quantum-emitter platform in hBN for free-space quantum networking and future integrated quantum-photonic architectures.

2D materials↗