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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 379 records · Page 21

Double photoionization of atomic oxygen: Feshbach resonances in the two-electron continuum

In this work, we describe a joint experimental and theoretical investigation on oxygen double photoionization—the emission of two electrons from atomic oxygen following single photon absorption. High-resolution experimental measurements were performed at the Advanced Light Source, revealing sharp resonance structure superimposed on the more familiar Wannier-like, nearly-linear background. These resonance features are attributed to ionization-plus-excitation Feshbach resonances embedded in the double ionization continuum, doubly-excited states that lie above the double-ionization threshold. Such features are absent in the double photoionization cross section of He, or other quasi-two-electron systems, for which the doubly-ionized atomic core remains inert. For a corresponding theoretical analysis, the R-matrix with pseudostates (RMPS) method was invoked by calculating final-state, two-electron resonances-plus-continua wavefunctions and corresponding single-photon absorption cross sections. Overall agreement is found in the direct, background double photoionization cross section. However, the RMPS method, using a small basis due to practical computational limitations, was unable to reproduce quantitatively the smooth background or the sharper resonance features observed in the measurements, showing instead large-scale oscillations about the experimental background, and characteristic pseudoresonance jitter, associated with an insufficient convergence of the pseudostate representation to the true two-electron infinite series of Feshbach resonances embedded in the two-electron continuum. The prominent resonance structure observed highlights the need to consider multiple excitation processes in atoms more complex than He or quasi-two-electron systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

Wide-Band, High-Quantum-Efficiency Photodetector

A design has been proposed for a photodetector that would exhibit a high quantum efficiency (as much as 90 percent) over a wide wavelength band, which would typically be centered at a wavelength of 1.55 m. This and similar photodetectors would afford a capability for detecting single photons - a capability that is needed for research in quantum optics as well as for the practical development of secure optical communication systems for distribution of quantum cryptographic keys. The proposed photodetector would be of the hot-electron, phonon-cooled, thin-film superconductor type. The superconducting film in this device would be a meandering strip of niobium nitride. In the proposed photodetector, the quantum efficiency would be increased through incorporation of optiA design has been proposed for a photodetector that would exhibit a high quantum efficiency (as much as 90 percent) over a wide wavelength band, which would typically be centered at a wavelength of 1.55 m. This and similar photodetectors would afford a capability for detecting single photons - a capability that is needed for research in quantum optics as well as for the practical development of secure optical communication systems for distribution of quantum cryptographic keys. The proposed photodetector would be of the hot-electron, phonon-cooled, thin-film superconductor type. The superconducting film in this device would be a meandering strip of niobium nitride. In the proposed photodetector, the quantum efficiency would be increased through incorporation of opti-

Jackson, Deborah↗

Probing dark exciton navigation through a local strain landscape in a WSe2 monolayer

Abstract In WSe 2 monolayers, strain has been used to control the energy of excitons, induce funneling, and realize single-photon sources. Here, we developed a technique for probing the dynamics of free excitons in nanoscale strain landscapes in such monolayers. A nanosculpted tapered optical fiber is used to simultaneously generate strain and probe the near-field optical response of WSe 2 monolayers at 5 K. When the monolayer is pushed by the fiber, its lowest energy states shift by as much as 390 meV (>20% of the bandgap of a WSe 2 monolayer). Polarization and lifetime measurements of these red-shifting peaks indicate they originate from dark excitons. We conclude free dark excitons are funneled to high-strain regions during their long lifetime and are the principal participants in drift and diffusion at cryogenic temperatures. This insight supports proposals on the origin of single-photon sources in WSe 2 and demonstrates a route towards exciton traps for exciton condensation.

36 MATERIALS SCIENCE↗

Giant optical second- and third-order nonlinearities at a telecom wavelength

A material platform that excels in both optical second- and third-order nonlinearities at a telecom wavelength is theoretically and experimentally demonstrated. In this TiN-based coupled metallic quantum well structure, electronic subbands are engineered to support doubly resonant inter-subband transitions for an exceptionally high second-order nonlinearity and provide single-photon transitions for a remarkable third-order nonlinearity within the 1400–1600 nm bandwidth. The second-order susceptibility χ (2) reaches 2840 pm/V at 1440 nm, while the Kerr coefficient n 2 arrives at 2.8 × 10 −10 cm 2 /W at 1460 nm. The achievement of simultaneous strong second- and third-order nonlinearities in one material at a telecom wavelength creates opportunities for multi-functional advanced applications in the field of nonlinear optics.

Chen, Ching-Fu (ORCID:0000000262510722)↗

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↗

Enhancing strontium clock atom interferometry using quantum optimal control

Strontium clock atom interferometry is a promising new technology, with multiple experiments under development around the world to explore its potential for dark matter and gravitational wave detection. In these detectors, large momentum transfer using sequences of many laser pulses is necessary, and thus high-fidelity pulses are important since small errors become magnified. Quantum optimal control (QOC) is a framework for developing control pulse waveforms that achieve high fidelity and are robust against experimental imperfections. Resonant single-photon transitions using the narrow clock transition of strontium involve significantly different quantum dynamics than more established atom interferometry methods based on far-detuned two-photon Raman or Bragg transitions, which leads to new opportunities and challenges when applying QOC. Here, we study in simulation QOC pulses for strontium clock interferometry and demonstrate their advantage over basic square pulses (primitive pulses) and composite pulses in terms of robustness against multiple noise channels. In conclusion, this could improve the scale of large momentum transfer in Sr clock interferometers, paving the way to achieving these scientific goals.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Patterned anodes with sub-millimeter spatial resolution for large-area MCP-based photodetector systems

Micro-channel-plate-based photo-detectors are unique in being capable of covering very large areas such as those required in elementary particle and nuclear physics, while providing sub-millimeter space resolution, time resolutions of less than 10 picoseconds for charged particles, and time resolutions of 30 psec–50 psec for single photons. In such systems the electronic channel count is a major cost driver. Incorporating a capacitively-coupled anode allows the use of external pickup electrodes with patterns of individual channels optimized for occupancy, rate, and time/space resolution. The signal pickup antenna can be economically implemented as a printed circuit card with a 2-dimensional array of pads for high-occupancy/high-rate applications such as in particle colliders and medical imaging, or a 1-dimensional array of strips for a lower channel count in low-occupancy/low-rate applications such as large neutrino detectors. In this paper we present pad patterns that enhance signal-sharing between pads to lower the channel count per unit area in large-area systems by factors up to 4, while maintaining spatial resolutions of approximately 100 to 200 μ m for charged particles and 400 to 1000 μ m for single photons. Patterns that use multiple signal layers in the signal-pickup board can lower the channel count even further, moving the scaling behavior in the number of pads versus total area from quadratic to linear.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Accelerating Quantum Materials Development with Advances in Transmission Electron Microscopy

Quantum materials are driving a technology revolution in sensing, communication, and computing, while simultaneously testing many core theories of the past century. Materials such as topological insulators, complex oxides, superconductors, quantum dots, color center-hosting semiconductors, and other types of strongly correlated materials can exhibit exotic properties such as edge conductivity, multiferroicity, magnetoresistance, superconductivity, single photon emission, and optical-spin locking. These emergent properties arise and depend strongly on the material’s detailed atomic-scale structure, including atomic defects, dopants, and lattice stacking. In this review, we describe how progress in the field of electron microscopy (EM), including in situ and in operando EM, can accelerate advances in quantum materials and quantum excitations. We begin by describing fundamental EM principles and operation modes. We then discuss various EM methods such as (i) EM spectroscopies, including electron energy loss spectroscopy (EELS), cathodoluminescence (CL), and electron energy gain spectroscopy (EEGS); (ii) four-dimensional scanning transmission electron microscopy (4D-STEM); (iii) dynamic and ultrafast EM (UEM); (iv) complementary ultrafast spectroscopies (UED, XFEL); and (v) atomic electron tomography (AET). We describe how these methods could inform structure–function relations in quantum materials down to the picometer scale and femtosecond time resolution, and how they enable precision positioning of atomic defects and high-resolution manipulation of quantum materials. For each method, we also describe existing limitations to solve open quantum mechanical questions, and how they might be addressed to accelerate progress. Among numerous notable results, our review highlights how EM is enabling identification of the 3D structure of quantum defects; measuring reversible and metastable dynamics of quantum excitations; mapping exciton states and single photon emission; measuring nanoscale thermal transport and coupled excitation dynamics; and measuring the internal electric field and charge density distribution of quantum heterointerfaces- all at the quantum materials’ intrinsic atomic and near atomic-length scale. Finally, we conclude by describing open challenges for the future, including achieving stable sample holders for ultralow temperature (below 10K) atomic-scale spatial resolution, stable spectrometers that enable meV energy resolution, and high-resolution, dynamic mapping of magnetic and spin fields. With atomic manipulation and ultrafast characterization enabled by EM, quantum materials will be poised to integrate into many of the sustainable and energy-efficient technologies needed for the 21st century.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Resolving Wave-Particle Duality Could Accelerate the Mass Production of Quantum Computers

Quantum computers, hypothesized in 1980s, use concepts of superposition and entanglement phenomena. Although theoretical propositions and associated search algorithms for accurate measurements are being generated, the development of practical quantum computers themselves are advancing very slowly requiring enormous time and investments. The underlying concepts of a quantum computer are not new to the optical domain. However, the crucial enabling concepts of Entanglement and Superposition Principle are remaining clouded under the unresolved postulates, Wave-Particle Duality (WPD), and Wave Packet Reduction (WPR), implicating incompleteness in the interpretations of the mathematical formalism behind Quantum Mechanics. The WPD debate started during late1600 between Newton and Huygens. Young’s resolution of WPD through his double-slit experiment in 1802 was effectively overturned by Einstein’s interpretation of photoelectric effect as due to “indivisible light quanta”. However, Einstein disowned his “light quanta” postulate shortly before his death in1955, even though it had earned him the Nobel Prize. We resolve WPD by synthesizing Newton’s and Maxwell’s concepts and assume atoms do emit quanta but propagate as time-finite exponential pulses. This assumption also resolves WPR for light-matter interaction with the assumption that Schrodinger’s ψ represents atom’s internal dipolar amplitude stimulations. This over-turns Born’s interpretation that ψ only represents the abstract mathematical probability amplitude, rather than the physical “internal amplitude stimulation” of the quantum entity. However, our concept of atomic pulse emission forces us to re-derive the expression for the N-slit grating-spectrometer response since the classical derivation uses CW light, which does not exist. This pulsespectrometric response function strengthens our postulate since the grating response to the exponential pulse appears to be the convolution of a Lorentzian spectrum with the classical CW response function of the grating. The Fourier Transform of an exponential function is Lorentzian and QM predicts spontaneous emission line width to be Lorentzian. Then, conceptually one can extend the grating-expression (with N=2) to get the double-slit pattern. This approach preserves the classical causality that each of the two slits, like the N-signals out of a grating, are physically real and jointly stimulate the quantum detector array at the far field to generate the “Local” cosine fringes. The detector array executes the square modulus operation on its imposed dipolar amplitude stimulation and absorbs the necessary energy to fill up their quantum cups. Hence the double-slit pattern must also be “Local”, just as the N-slit grating spectrum is generated locally at the exit spectral-plane of the spectrometer. This removes the need to believe that “single photons” mysteriously generate the double slit pattern. Quantum computers, hypothesized in 1980s, use concepts of superposition and entanglement phenomena. Although theoretical propositions and associated search algorithms for accurate measurements are being generated, the development of practical quantum computers themselves are advancing very slowly requiring enormous time and investments. The underlying concepts of a quantum computer are not new to the optical domain. However, the crucial enabling concepts of Entanglement and Superposition Principle are remaining clouded under the unresolved postulates, Wave-Particle Duality (WPD), and Wave Packet Reduction (WPR), implicating incompleteness in the interpretations of the mathematical formalism behind Quantum Mechanics. The WPD debate started during late1600 between Newton and Huygens. Young’s resolution of WPD through his double-slit experiment in 1802 was effectively overturned by Einstein’s interpretation of photoelectric effect as due to “indivisible light quanta”. However, Einstein disowned his “light quanta” postulate shortly before his death in1955, even though it had earned him the Nobel Prize. We resolve WPD by synthesizing Newton’s and Maxwell’s concepts and assume atoms do emit quanta but propagate as time-finite exponential pulses. This assumption also resolves WPR for light-matter interaction with the assumption that Schrodinger’s ψ represents atom’s internal dipolar amplitude stimulations. This over-turns Born’s interpretation that ψ only represents the abstract mathematical probability amplitude, rather than the physical “internal amplitude stimulation” of the quantum entity. However, our concept of atomic pulse emission forces us to re-derive the expression for the N-slit grating-spectrometer response since the classical derivation uses CW light, which does not exist. This pulsespectrometric response function strengthens our postulate since the grating response to the exponential pulse appears to be the convolution of a Lorentzian spectrum with the classical CW response function of the grating. The Fourier Transform of an exponential function is Lorentzian and QM predicts spontaneous emission line width to be Lorentzian. Then, conceptually one can extend the grating-expression (with N=2) to get the double-slit pattern. This approach preserves the classical causality that each of the two slits, like the N-signals out of a grating, are physically real and jointly stimulate the quantum detector array at the far field to generate the “Local” cosine fringes. The detector array executes the square modulus operation on its imposed dipolar amplitude stimulation and absorbs the necessary energy to fill up their quantum cups. Hence the double-slit pattern must also be “Local”, just as the N-slit grating spectrum is generated locally at the exit spectral-plane of the spectrometer. This removes the need to believe that “single photons” mysteriously generate the double slit pattern.

Quantum Computer↗

First-principles study of the Stark shift effect on the zero-phonon line of the NV center in diamond

Point defects in semiconductors are attractive candidates for quantum information science applications owing to their ability to act as spin-photon interface or single-photon emitters. However, the coupling between the change of dipole moment upon electronic excitation and stray electric fields in the vicinity of the defect, an effect known as Stark shift, can cause significant spectral diffusion in the emitted photons. In this work, using first principles computations, we revisit the methodology to compute the Stark shift of point defects up to the second order. The approach consists of applying an electric field on a defect in a slab and monitoring the changes in the computed zero-phonon line (i.e., difference in energy between the ground and excited state) obtained from constraining the orbital occupations (constrained-DFT). Here, we study the Stark shift of the negatively charged nitrogen-vacancy (NV) center in diamond using this slab approach. We discuss and compare two approaches to ensure a negatively charged defect in a slab and we show that converged values of the Stark shift measured by the change in dipole moment between the ground and excited states (Δ⁢μ) can be obtained. We obtain a Stark shift of Δ⁢μ = 2.68⁢D using the semilocal GGA-PBE functional and of Δ⁢μ = 2.23⁢D using the HSE hybrid functional. These values are in good agreement with experimental results. We also show that modern theory of polarization can be used on constrained-DFT to obtain Stark shifts in very good agreement with the slab computations.

36 MATERIALS SCIENCE↗

Quantum-Enhanced Sensing of Axion Dark Matter with a Transmon-Based Single Microwave Photon Counter

We report an axion dark matter search with a haloscope equipped with a microwave photon counter. The haloscope is a tunable high quality factor three-dimensional microwave cavity placed in a magnetic field. The photon counter, operated cyclically, maps an incoming microwave photon onto the state of a superconducting transmon qubit. The measurement protocol continuously monitors the power emitted by the haloscope cavity as well as the dark count background and enables tuning of the cavity frequency to probe different axion masses. With this apparatus, we enhance by a factor of 20 the search speed that can be reached with quantum-limited linear amplifiers and set a new standard for probing the existence of axions with resonant detectors above 5 GHz. Published by the American Physical Society 2025

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Quantum Imaging with X-rays

Quantum imaging encompasses a broad range of methods that exploit the quantum properties of light to capture information about an object. One such approach involves using a two-photon quantum state, where only one photon interacts with the object being imaged while its entangled partner carries spatial or temporal information. To implement this technique, it is necessary to generate specific quantum states of light and detect photons at the single-photon level. While this method has been successfully demonstrated in the visible electromagnetic spectrum, extending it to X-rays has faced significant challenges due to the difficulties in producing a sufficient rate of X-ray photon pairs and detecting them with adequate resolution. Here, we demonstrate record high rates of correlated X-ray photon pairs produced via a spontaneous parametric down-conversion process and we employ these photons to perform quantum correlation imaging of several objects, including a biological sample (E. cardamomum seedpod). Notably, we report an unprecedented detection rate of about 6,300 pairs per hour and the observation of energy anti-correlation for the X-ray photon pairs. We also present a detailed analysis of the properties of the down-converted X-ray photons, as well as a comprehensive study of the correlation imaging formation, including a study of distortions and corrections. These results mark a substantial advancement in X-ray quantum imaging, expanding the possibilities of X-ray quantum optical technologies, and illustrating the pathway towards enhancing biological imaging with reduced radiation doses.

Gofron, Kaz [ORNL] (ORCID:0000000314415736)↗

Simultaneous Two- and Three-Photon Deep Imaging of Autofluorescence in Bacterial Communities

The intrinsic fluorescence of bacterial samples has a proven potential for label-free bacterial characterization, monitoring bacterial metabolic functions, and as a mechanism for tracking the transport of relevant components through vesicles. The reduced scattering and axial confinement of the excitation offered by multiphoton imaging can be used to overcome some of the limitations of single-photon excitation (e.g., scattering and out-of-plane photobleaching) to the imaging of bacterial communities. In this work, we demonstrate in vivo multi-photon microscopy imaging of Streptomyces bacterial communities, based on the excitation of blue endogenous fluorophores, using an ultrafast Yb-fiber laser amplifier. Its parameters, such as the pulse energy, duration, wavelength, and repetition rate, enable in vivo multicolor imaging with a single source through the simultaneous two- and three-photon excitation of different fluorophores. Three-photon excitation at 1040 nm allows fluorophores with blue and green emission spectra to be addressed (and their corresponding ultraviolet and blue single-photon excitation wavelengths, respectively), and two-photon excitation at the same wavelength allows fluorophores with yellow, orange, or red emission spectra to be addressed (and their corresponding green, yellow, and orange single-photon excitation wavelengths). We demonstrate that three-photon excitation allows imaging over a depth range of more than 6 effective attenuation lengths to take place, corresponding to an 800 micrometer depth of imaging, in samples with a high density of fluorescent structures.

59 BASIC BIOLOGICAL SCIENCES↗

Inelastic Scattering of a Photon by a Quantum Phase Slip

Spontaneous decay of a single photon is a notoriously inefficient process in nature irrespective of the frequency range. We report that a quantum phase-slip fluctuation in high-impedance superconducting waveguides can split a single incident microwave photon into a large number of lower-energy photons with a near unit probability. The underlying inelastic photon-photon interaction has no analogs in non-linear optics. Instead, the measured decay rates are explained without adjustable parameters in the framework of a new model of a quantum impurity in a Luttinger liquid. Our result connects circuit quantum electrodynamics to critical phenomena in two-dimensional boundary quantum field theories, important in the physics of strongly-correlated systems. Here, the photon lifetime data represents a rare example of verified and useful quantum many-body simulation.

1-dimensional systems↗

Generation of Antibunched Light by Excited Molecules in a Microcavity Trap

The active microcavity is adopted as an efficient source of non-classical light. By this device, excited by a mode-locked laser at a rate of 100 MHz, single-photons are generated over a single field mode with a nonclassical sub-poissonian distribution. The process of adiabatic recycling within a multi-step Franck-Condon molecular optical-pumping mechanism, characterized in our case by a quantum efficiency very close to one, implies a pump self-regularization process leading to a striking n-squeezing effect. By a replication of the basic single-atom excitation process a beam of quantum photon (Fock states) can be created. The new process represents a significant advance in the modern fields of basic quantum-mechanical investigation, quantum communication and quantum cryptography.

DeMartini, F.↗