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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 127 records · Page 7

Spin-Controllable Dynamics in Defect-Engineered Carbon Nanotubes as Single Photon Emitters: Data-Driven Modeling and Computations

Quantum technologies, such as quantum computing and sensing, require efficient single-photon emission (SPE) sources that operate at room temperature in telecom wavelengths. While several materials can serve as SPE sources, no single platform meets all the criteria for efficiency, ambient operation, and scalability. Single-walled carbon nanotubes (SWCNTs) with covalently attached molecules offer a promising solution. Their SPE can be easily tuned via modifications of the SWCNT's diameter, chirality, and bonded molecules, enabling emission across near-IR to telecom wavelengths at ambient conditions. However, to fully realize the potential of SWCNTs and unlock their quantum capabilities, a deeper understanding of how structural defects from molecular adducts affect their emission and competing photoexcited processes is essential. To address this gap in our knowledge, this project combined quantum chemistry calculations with data-driven methods of cheminformatics (QSAR) and machine learning (ML). The developed computational approaches have provided several design strategies for covalent functionalization of SWCNTs to improve their optical response. The collaboration with Los Alamos National Lab (LANL) enabled direct comparison of computational and experimental data, facilitating method validation. This partnership was enhanced through access to LANL's Center for Integrated Nanotechnologies (CINT) utilizing User Facility Program and summer internships, which provided three NDSU graduate students with hands-on experience at LANL. The outcomes of this project included (1) Advancing the current stage of computational methods in accurate modeling of non-adiabatic spin-dependent photoexcited dynamics and its applicability to nanosystems consisting of thousands of atoms, realized as open-access codes linked to existing DFT-based software; (2) Establishing the relationship between the structure of adducts and SWCNTs and intrinsic excitonic and spin properties of defect states for guiding novel synthetic strategies and experimental probes of chemically functionalized SWCNTs as near-IR emitting materials; (3) Generating virtual libraries of hypothetical functionalized SWCNTs for virtual screening of their chemical structures and optical properties, leveraging new functionalities of SWCNTs; (4) Offering a unique experience for NDSU graduate students that prepared them for future scientific careers related to materials modeling and big data processing. These results were summarized in 12 published journal papers and 3 recently submitted papers. One of a key finding is that the position of defect sites on the SWCNT surface primarily drives the emission redshift (up to 100 meV), while the polarity of the defect-inducing molecules has a much smaller effect (~10 meV). However, the electron-donating or withdrawing properties of a molecule influence selecting reactivity of defect sites. These insights important for optimizing synthetic protocols for desired emissions in SWCNTs. We also revealed that the interaction between two defects at various positions on the SWCNT enhances the redshift and optical activity of states, favoring strong near-IR emission. This suggests that manipulations in defect concentrations is a promising strategy for controlling efficient emission. Mostly important, the defect position was found controllable by the spin states of photoexcited intermediates: Excited aromatic molecules form ortho defects with SWCNTs at their singlet states in the presence of oxygen, while oxygen-free conditions favor para defects via the triplet-state mechanism. Additionally, a heat-activated [2+2] cycloaddition reaction facilitates divalent defect formation with fewer bonding positions that narrows emission bands. These groundbreaking findings have been experimentally validated and significantly advance our understanding of defect chemistry in SWCNTs. Using a novel encoding technique and 3D-MoRSE descriptors, we developed highly accurate ML/QSAR models to predict both the 3D structure and optical properties of SWCNTs with chemical defects. This model enabled the creation of a virtual library of 125,556 structures, providing new insights into the relationship between SWCNT-defect structure and emission.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Deterministic Localization of Strain-Induced Single-Photon Emitters in Multilayer GaSe

The nanoscale strain has emerged as a powerful tool for controlling single-photon emitters (SPEs) in atomically thin transition metal dichalcogenides (TMDCs). However, quantum emitters in monolayer TMDCs are typically unstable in ambient conditions. Multilayer TMDCs could be a solution, but they suffer from low quantum efficiency, resulting in low brightness of the SPEs. Here, we report the deterministic spatial localization of strain-induced SPEs in multilayer GaSe by nanopillar arrays. The strain-controlled quantum confinement effect introduces well-isolated sub-bandgap photoluminescence and corresponding suppression of the broad band edge photoluminescence. Clear photon-antibunching behavior is observed from the quantum dot-like GaSe sub-bandgap exciton emission at 3.5 K. The strain-dependent confinement potential and the brightness are found to be strongly correlated, suggesting a promising route for tuning and controlling SPEs. The comprehensive investigations of strain-engineered GaSe SPEs provide a solid foundation for the development of 2D devices for quantum photonic technologies.

2D materials↗

HgCdTe e-APD Detector Arrays with Single Photon Sensitivity for Space Lidar Applications

A multi-element HgCdTe electron initiated avalanche photodiode (e-APD) array has been developed for space lidar applications. The detector array was fabricated with 4.3-μm cutoff HgCdTe which covered a spectral response from 0.4 to 4.3 μm. We have characterized a 4x4 detector array with 80 μm square elements and an integrated custom cryogenic silicon read-out integrated circuit (ROIC). The device operated at 77K inside a small closed-cycle Dewar. Measurements showed a unity gain quantum efficiency of about 90% at 1.55 μm. The bulk dark current of the HgCdTe e-APD at 77K was less than 50,000 input referred electrons/s at 12 V APD bias where the APD gain was 620 and the measured noise equivalent power (NEP) was 0.4 fW/Hz1/2. The electrical bandwidth of the ROIC was about 6 MHz, which was chosen to match the laser pulse width of our CO2 lidar. Even with the relatively low bandwidth, the high APD gain and low dark current enabled the device to detect single photon events. Because the APD was biased below the break-down voltage, the detector output was linear with the input optical signal and there was no dead-time and afterpulsing. A new series of HgCdTe e-APDs are being developed with a much wider bandwidth ROIC and higher gain HgCdTe e-APD array, which is expected to give a much better performance in linear mode photon counting applications.

HgCdTe↗

Few-Mode Fiber Coupled Superconducting Nanowire Single-Photon Detectors for Photon Efficient Optical Communications

The NASA Glenn Research Center's development of a high-photon efficiency real-time optical communications ground receiver has added superconducting nanowire single-photon detectors (SNSPDs) coupled with few-mode fibers (FMF). High data rate space-to-ground optical communication links require enhanced ground receiver sensitivity to reduce spacecraft transmitter constraints, and therefore require highly efficient coupling from fiber to detector. In the presence of atmospheric turbulence the received optical wave front can be severely distorted introducing higher-order spatial mode components to the received signal. To reduce mode filtering and mismatch loss and the resulting degradations to detector coupling efficiency, we explore the use of few-mode fiber coupling to commercial single-pixel SNSPDs. Graded index 20-µm few-mode fibers allow the commercial single pixel SNSPD's active area to couple with equal efficiency as single mode fibers. Here we determine detector characteristics such as count rate, detection efficiency, dark counts, and jitter, as well as detection efficiencies for higher-order fiber spatial modes. Additionally, we assess the laboratory performance of the detectors in an optical system which emulates future deep space optical communications links.

Vyhnalek, Brian E.↗

Comparing photosynthetic light harvesting of single photons and pseudothermal light under ultraweak illumination

Photosynthesis in vivo is driven by sunlight, an ultraweak incoherent thermal source. However, most experiments and theories have studied photosynthetic light harvesting driven by strong coherent laser sources. The quantum states of light are characterized by their photon statistics, in addition to classical properties such as intensity and frequency spectrum. Here, we report experiments that investigate how photon statistics affect a natural photosynthetic system and vice versa. We directly compare how single photons and pseudothermal light from spontaneous parametric down-conversion drive light harvesting in the light-harvesting 2 complex from a purple bacterium. We find that the fluorescence lifetime and quantum efficiency are unchanged while the fluorescence photon statistics are markedly different, resembling that of the incident light, implying that the dynamics do not fundamentally modify the photon statistics. This represents a step toward clarification of the similarities and differences between photosynthetic light harvesting in laboratory and in natural sunlight conditions.

Li, Quanwei [University of California, Berkeley, C↗

Single photon infrared emission spectroscopy: a study of IR emission from UV laser excited PAHs between 3 and 15 micrometers

Single-photon infrared emission spectroscopy (SPIRES) has been used to measure emission spectra from polycyclic aromatic hydrocarbons (PAHs). A supersonic free-jet expansion has been used to provide emission spectra of rotationally cold and vibrationally excited naphthalene and benzene. Under these conditions, the observed width of the 3.3-micrometers (C-H stretch) band resembles the bandwidths observed in experiments in which emission is observed from naphthalene with higher rotational energy. To obtain complete coverage of IR wavelengths relevant to the unidentified infrared bands (UIRs), UV laser-induced desorption was used to generate gas-phase highly excited PAHs. Lorentzian band shapes were convoluted with the monochromator-slit function in order to determine the widths of PAH emission bands under astrophysically relevant conditions. Bandwidths were also extracted from bands consisting of multiple normal modes blended together. These parameters are grouped according to the functional groups mostly involved in the vibration, and mean bandwidths are obtained. These bandwidths are larger than the widths of the corresponding UIR bands. However, when the comparison is limited to the largest PAHs studied, the bandwidths are slightly smaller than the corresponding UIR bands. These parameters can be used to model emission spectra from PAH cations and cations of larger PAHs, which are better candidate carriers of the UIRs.

Non-NASA Center↗

Preliminary results from a single-photon imaging X-ray charge coupled device /CCD/ camera

A CCD camera is described which has been designed for single-photon X-ray imaging in the 1-10 keV energy range. Preliminary results are presented from the front-side illuminated Fairchild CCD 211, which has been shown to image well at 3 keV. The problem of charge-spreading above 4 keV is discussed by analogy with a similar problem at infrared wavelengths. The total system noise is discussed and compared with values obtained by other CCD users.

Griffiths, R. E.↗

Systems, methods, and media for high dynamic range imaging using single-photon and conventional image sensor data

In accordance with some embodiments, systems, methods, and media for high dynamic range imaging using single-photon and conventional image sensor data are provided. In some embodiments, the system comprises: first detectors configured to detect a level of photons proportional to incident photon flux; second detectors configured to detect arrival of individual photons; a processor programmed to: receive, from the first detectors, first values indicative of photon flux from a scene with a first resolution; receive, from the second detectors, second values indicative of photon flux from the scene with a lower resolution; provide a first encoder of a trained machine learning model first flux values based on the first values, provide the second encoder of the model second flux values; receive, as output, values indicative of photon flux from the scene; and generate a high dynamic range image based on the third plurality of values.

Gutierrez Barragan, Felipe↗

Search for anomalous neutral current coherent-like single-photon production in MicroBooNE

MicroBooNE is a liquid argon time projection chamber (TPC) detector which offers excellent spatial and energy resolution and the ability to distinguish electrons from photons. In this note we present preliminary results from a dedicated search for neutral current (NC) single-photon production, with a focus on forward-going photons and no visible hadronic activity, both of which are key characteristics of “coherent-like” electromagnetic shower production. A total efficiency for SM-predicted NC coherent 1γ events of 12.5% is obtained, defined relative to simulated events in the entire MicroBooNE active TPC. Relative to the Pandora-reconstructed single-shower event selection, the analysis achieves a 95% rejection of non-coherent NC 1π 0 background events and a 99.97% rejection of cosmic background events, while maintaining a signal efficiency of approximately 45%.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Search for Anomalous Neutral Current Coherent-Like Single-Photon Production in MicroBooNE

MicroBooNE is a liquid argon time projection chamber (TPC) detector which offers excellent spatial and energy resolution and the ability to distinguish electrons from photons. In this note we present preliminary results from a dedicated search for neutral current (NC) single-photon production, with a focus on forward-going photons and no visible hadronic activity, both of which are key characteristics of “coherent-like” electromagnetic shower production. A total efficiency for SM-predicted NC coherent 1$\gamma$ events of 12.5% is obtained, defined relative to simulated events in the entire MicroBooNE active TPC. Relative to the Pandora-reconstructed single-shower event selection, the analysis achieves a 95% rejection of non-coherent NC 1π 0 background events and a 99.97% rejection of cosmic background events, while maintaining a signal efficiency of approximately 45%.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Strongly coupled intermediate electronic states in one-color two-photon single valence ionization of O 2

Here, we present an experimental and theoretical energy- and angle-resolved investigation on the non-dissociative photoionization dynamics of near-resonant, one-color, two-photon, single valence ionization of neutral O 2 molecules. Using 9.3 eV femtosecond pulses produced via high harmonic generation and a 3-D momentum imaging spectrometer, we detect the photoelectrons and O$^{+}_{2}$ cations produced from one-color, two-photon ionization in coincidence. The measured and calculated photoelectron angular distributions show agreement, which indicates that a superposition of two intermediate electronic states is dominantly involved and that wavepacket motion on those near-resonantly populated intermediate states does not play a significant role in the measured two-photon ionization dynamics. Here, we find greater utility in the diabatic representation compared to the adiabatic representation, where invoking a single valence-character diabat is sufficient to describe the underlying two-photon ionization mechanism.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Search for new physics in the final state with a single photon and large missing transverse momentum in proton-proton collisions at √𝑠 =13 TeV

A search for new physics in events featuring a single photon and missing transverse momentum is presented, using proton-proton √𝑠 =13 TeV collision data corresponding to an integrated luminosity of 101 fb −1 collected by the CMS experiment at the CERN LHC between 2017 and 2018. This analysis, combined with a previous study of 36 fb −1 of 2016 data (totaling 137 fb −1 ), reveals no significant deviations from standard model expectations. The results are then used to establish 95% confidence level limits on parameters in theoretical models involving dark matter and large extra dimensions. Compared to the 2016-only analysis, this search achieves up to a 14% improvement in exclusion reach for mediator masses in simplified dark matter models, along with 11% and 10% enhancements in the limits on the effective field theory suppression scale and the fundamental Planck scale, respectively. These results are the most stringent constraints on these parameters to date.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Mechanisms and dynamics of the NH + 2 + H + and NH + + H + + H fragmentation channels upon single-photon double ionization of NH 3

We present state-selective measurements on the NH$_2^{+}$ + H$^{+}$ and NH$^{+}$ + H$^{+}$ + H dissociation channels following single-photon double ionization at 61.5 eV of neutral NH$_{3}$, where the two photoelectrons and two cations are measured in coincidence using 3-D momentum imaging. Three dication electronic states are identified to contribute to the NH$_2^{+}$ + H$^{+}$ dissociation channel, where the excitation in one of the three states undergoes intersystem crossing prior to dissociation, producing a cold NH$_2^+$ fragment. In contrast, the other two states directly dissociate, producing a ro-vibrationally excited NH$_2^+$ fragment with roughly 1 eV of internal energy. The NH$^{+}$ + H$^{+}$ + H channel is fed by direct dissociation from three intermediate dication states, one of which is shared with the NH$_2^{+}$ + H$^{+}$ channel. We find evidence of autoionization contributing to each of the double ionization channels. Finally, the distributions of the relative emission angle between the two photoelectrons, as well as the relative angle between the recoil axis of the molecular breakup and the polarization vector of the ionizing field, are also presented to provide insight on the ionization mechanisms for the different dication states.

74 ATOMIC AND MOLECULAR PHYSICS↗

High-Fidelity Down-Conversion Source for Secure Communications Using On-Demand Single Photons

AdvR, Inc., has built an efficient, fully integrated, waveguide-based source of spectrally uncorrelated photon pairs that will accelerate research and development (R&D) in the emerging field of quantum information science. Key to the innovation is the use of submicron periodically poled waveguides to produce counter propagating photon pairs, which is enabled by AdvR's patented segmented microelectrode poling technique. This novel device will provide a high brightness source of down-conversion pairs with enhanced spectral properties and low attenuation, and it will operate in the visible to the mid-infrared spectral region. A waveguide-based source of spectrally and spatially pure heralded photons will contribute to a wide range of NASA's advanced technology development efforts, including on-demand single photon sources for high-rate spaced-based secure communications.

Roberts, Tony↗

Experimental tests of a single-photon calorimeter for X-ray spectroscopy

Tests have been made of a nondispersive spectroscopic X-ray detector which operates by measuring the temperature rise following absorption of a single photon. Thermal pulses from 6-keV X-rays have been observed, and the different amplitudes resulting from Mn K-alpha and K-beta events have been resolved. This device was assembled to make quantitative tests of theoretical calculations of the properties of such detectors, and its high heat capacity does not allow it to attain the very high resolution predicted for detectors made by more sophisticated, but still straightforward, techniques. Both the measured resolution of 270-eV full width at half maximum and the absolute amplitude of the response are consistent with predictions. Nonthermal effects in the thermistor limit the precision of this comparison to about 30 percent.

Mccammon, D.↗

High-dimensional quantum key distribution using orbital angular momentum of single photons from a colloidal quantum dot at room temperature

High-dimensional quantum key distribution (HDQKD) is a promising avenue to address the inherent limitations of basic quantum key distribution (QKD) protocols. However, experimental realizations of HDQKD to date have relied on indeterministic photon sources that limit the achievable key rate. In this paper, we demonstrate a full emulation of a HDQKD system using a single colloidal giant quantum dot (gQD) as a deterministic, compact, and room-temperature single-photon source (SPS). We demonstrate a practical protocol by encoding information in a high-dimensional space (d = 3) of the orbital angular momentum of the photons. Our experimental configuration incorporates two spatial light modulators for encoding and decoding the spatial information carried by individual photons. Our experimental demonstration establishes the feasibility of utilizing high radiative quantum yield gQDs as practical SPSs for HDQKD. We also experimentally demonstrate surpassing the traditional d = 2 QKD capacity with comparable error rates, indicating a significant improvement in performance while maintaining reliability.

36 MATERIALS SCIENCE↗