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DOE OSTI2025

Telecom-Wavelength Single-Photon Emitters in Multilayer InSe

The development of robust and efficient single-photon emitters (SPEs) at telecom wavelengths is critical for advancements in quantum information science. Two-dimensional (2D) materials have recently emerged as promising sources for SPEs, owing to their high photon extraction efficiency, facile coupling to external fields, and seamless integration into photonic circuits. In this study, we demonstrate the creation of SPEs emitting in the 1000–1550 nm near-infrared range by coupling 2D indium selenide (InSe) with strain-inducing nanopillar arrays. The emission wavelength exhibits a strong dependence on the number of layers. Hanbury Brown and Twiss experiments conducted at 10 K reveal clear photon antibunching, confirming the single-photon nature of the emissions. In conclusion, density-functional-theory calculations and scanning-tunneling-microscopy analyses provide insights into the electronic structures and defect states, elucidating the origins of the SPEs.

2D Material↗

DOE OSTI2020

Single-pulse (100 ps) extended x-ray absorption fine structure capability at the Dynamic Compression Sector

Determining real-time changes in the local atomistic order is important for a mechanistic understanding of shock wave induced structural and chemical changes. However, the single event and short duration (nanosecond times) nature of shock experiments pose challenges in obtaining Extended X-ray Absorption Fine Structure (EXAFS) measurements - typically used for monitoring local order changes. Here, we report on a new single pulse (~100 ps duration) transmission geometry EXAFS capability for use in laser shock-compression experiments at the Dynamic Compression Sector (DCS), Advanced Photon Source. We used a flat plate of highly oriented pyrolytic graphite (HOPG) as the spectrometer element to energy disperse x-rays transmitted through the sample. It provided high efficiency with approximately 15% of the x-rays incident on the HOPG reaching an x-ray area detector with high quantum efficiency. This combination resulted in good signal-to-noise ratio (~10 3 ), energy resolution of ~10 eV at 10 keV, EXAFS spectra covering 100s of eV, and good pulse to pulse reproducibility of our single pulse measurements. Ambient EXAFS spectra for Cu and Au are compared to reference spectra, validating our measurement system. Comparison of single pulse EXAFS results for ambient and laser shocked Ge(100) shows large changes to the local structure of the short lived state of shocked Ge. The current DCS EXAFS capability can be used to perform single pulse measurements in laser shocked materials from approximately 9-13 keV. These EXAFS developments will be available to all users of the DCS.

47 OTHER INSTRUMENTATION↗

NASA NTRS1971

Long term temporal variations of the hard X-ray flux from the Centaurus region

The X-ray telescope aboard the third Orbiting Solar Observatory (OSO-3) observed the Centaurus region daily from 1967 October to 1968 February, and also for five days in 1968 June. A stable minimum flux of 0.33 + or - 0.03 photons (sq cm sec)/1 between 7.7 and 38 keV from a source around l = 305 deg is derived. Several single days show enhanced fluxes, and two extensive flaring episodes, one with a soft and the other a very hard spectrum, lasting at least ten days.

Schwartz, D. A.↗

DOE OSTI2025

Dirhodium(II,II) Complexes as Panchromatic Single-Molecule Photocatalysts for Hydrogen Evolution

The growing global energy demand and climate change have prompted a shift from carbon-based fuels to sustainable energy sources. Hydrogen production by harnessing solar energy and using abundant proton sources represents an attractive approach to addressing this crisis. Single-molecule single-chromophore photocatalysts, capable of both absorbing the incident photon and catalyzing the chemical transformation, are able to circumvent energy losses present in multicomponent systems that require a photosensitizer and a catalyst, often employing additional redox relay molecules. Here, the series of complexes derived from cis-[Rh 2 (μ-DPhF) 2 (μ-bncn) 2 ] 2+ (1; DPhF = N,N′-diphenylformamidinate, bncn = benzo[c]cinnoline) discussed in this Account presents robust and air-stable single-molecule photocatalysts with panchromatic absorption from the ultraviolet spectral region to the near-infrared (NIR), with high turnover frequencies of ∼20 to 30 h –1 under red light irradiation. For comparison, other single-molecule hydrogen-evolving photocatalysts reported to date exhibit low photocatalytic efficiency, are not operable in the visible or NIR regions, and are unstable under an ambient atmosphere.

Absorption↗

DOE OSTI2020

Second Harmonic Generation from a Single Plasmonic Nanorod Strongly Coupled to a WSe 2 Monolayer

Monolayer transition metal dichalcogenides, coupled to metal plasmonic nanocavities, have recently emerged as new platforms for strong light–matter interactions. These systems are expected to have nonlinear-optical properties that will enable them to be used as entangled photon sources, compact wave-mixing devices, and other elements for classical and quantum photonic technologies. Here, we report the first experimental investigation of the nonlinear properties of these strongly coupled systems, by observing second harmonic generation from a WSe 2 monolayer strongly coupled to a single gold nanorod. In this work, the pump-frequency dependence of the second-harmonic signal displays a pronounced splitting that can be explained by a coupled-oscillator model with second-order nonlinearities. Rigorous numerical simulations utilizing a nonperturbative nonlinear hydrodynamic model of conduction electrons support this interpretation and reproduce experimental results. Our study thus lays the groundwork for understanding the nonlinear properties of strongly coupled nanoscale systems.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

DOE OSTI2021

Bright, single helicity, high harmonics driven by mid-infrared bicircular laser fields

High-harmonic generation (HHG) is a unique tabletop light source with femtosecond-to-attosecond pulse duration and tailorable polarization and beam shape. Here, we use counter-rotating femtosecond laser pulses of 0.8 µm and 2.0 μm to extend the photon energy range of circularly polarized high-harmonics and also generate single-helicity HHG spectra. By driving HHG in helium, we produce circularly polarized soft x-ray harmonics beyond 170 eV—the highest photon energy of circularly polarized HHG achieved to date. In an Ar medium, dense spectra at photon energies well beyond the Cooper minimum are generated, with regions composed of a single helicity—consistent with the generation of a train of circularly polarized attosecond pulses. Finally, we show theoretically that circularly polarized HHG photon energies can extend beyond the carbon K edge, extending the range of molecular and materials systems that can be accessed using dynamic HHG chiral spectro-microscopies.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1983

EGRET - The high energy gamma ray telescope for NASA's Gamma Ray Observatory

The EGRET high energy gamma-ray telescope under development for NASA's Gamma Ray Observatory will have an energy range of approximately 12 to 30,000 MeV, energy resolution of about 15 percent FWHM over most of that range, an effective area of about 2000 sq cm at high energies, and single photon angular accuracy of approximately 2 deg at 100 MeV, less than 0.1 deg above 5 GeV. This instrument can locate strong sources to an accuracy of about 5 arc min. The instrument utilizes a set of digital spark chambers interleaved with tantalum foils for detection and identification of gamma-ray events, and a large NaI(Tl) scintillator for energy determination. The system is triggered by a coincidence matrix using two arrays of plastic scintillation counters and a large plastic scintillator anticoincidence dome that rejects incident charged particles.

Fichtel, C. E.↗

DOE OSTI2021

Radiation-Induced Dark Counts for Silicon Single-Photon Detectors in Space

Single-photon detectors operating on satellites for use in a quantum communications network can incur large dark-count-rate increases from the natural radiation environment of space. Displacement damage to the material lattice of a detector from the ionizing radiation can result in a permanent dark-count increase in the detector. In this work, we analyze the radiation-induced dark-count rate of a silicon single-photon avalanche diode onboard a satellite at different orbiting altitudes, as well as, the additional radiation from a nuclear-disturbed environment caused by a high-altitude nuclear explosion. For detectors on low Earth orbit satellites, protons are the biggest source of radiation damage and are best mitigated by choosing an orbit that minimizes exposure when passing through the South Atlantic Anomaly and Polar Cusps. Detectors on medium Earth orbit and geostationary orbit satellites, if shielded by more than 10 mm of aluminum, provide the best platform in terms of the least amount of radiation damage to the detectors. In the event of a high-altitude nuclear explosion, the artificial radiation belts produced by the explosion will cause too much damage to silicon single-photon detectors on low Earth orbit satellites and render them unfit for quantum communications in less than a day. Higher orbit satellites will only suffer minor dark-count-rate increases from the artificial radiation belts.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

NASA NTRS1972

Long-term temporal variations of the hard X-ray flux from the Centaurus region.

An X-ray telescope aboard OSO 3 observed the Centaurus region daily from October 1967 to February 1968, and also for five days in June 1968. For this period, we derive a stable minimum flux of 0.33 plus or minus 0.33 photons per sq cm per sec between 7.7 and 38 keV from a persistent hard X-ray source around 305 deg longitude. Several single days show enhanced fluxes; and two extensive flaring episodes, one with a soft and the other with a very hard spectrum, last at least 10 days.

Schwartz, D. A.↗

NASA NTRS1996

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.↗

DOE OSTI2020

Method for dynamic control of light emission from phosphors with heat excitations

An optically emissive material and, in particular, materials for use in single photon generation technologies, have multiple excited energy states that have different decay rates and can emit photons with different properties. A primary excitation radiation source is configured to apply primary radiation to an optically emissive material to excite the optically emissive material into a primary excited state. A secondary excitation radiation source is configured to apply secondary radiation to a thermal contribution material to generate thermal energy in the thermal contribution material. The thermal contribution material is physically configured to transfer thermal energy to the optically emissive material and excite the optically emissive material from the primary excited state to a secondary excited state for dynamic control of the emission rate, or emitted photon properties, of the optically emissive material.

36 MATERIALS SCIENCE↗

NASA NTRS2004

Gamma-ray Spectral Characteristics of Thermal and Non-thermal Emission from Three Black Holes

Cygnus X-1 and the gamma-ray transients GROJ0422+32 and GROJ1719-24 displayed similar spectral properties when they underwent transitions between the high and low gamma-ray (30 keV to few MeV) intensity states. When these sources were in the high (gamma)-ray intensity state ((gamma)2, for Cygnus X-l), their spectra featured two components: a Comptonized shape below 200-300 keV with a soft power-law tail (photon index >= 3) that extended to ~1 MeV or beyond. When the sources were in the low-intensity state ((gamma)0, for Cygnus X-l), the Comptonized spectral shape below 200 keV typically vanished and the entire spectrum from 30 keV to ~1 MeV can be characterized by a single power law with a relatively harder photon index ~2-2.7. Consequently the high- and low-intensity gamma-ray spectra intersect, generally in the ~400 KeV - ~1 MeV range, in contrast to the spectral pivoting seen previously at lower (~10 keV) energies. The presence of the power-law component in both the high- and low-intensity gammaray spectra strongly suggests that the non-thermal process is likely to be at work in both the high and the low-intensity situations. We have suggested a possible scenario (Ling & Wheaton, 2003), by combining the ADAF model of Esin et al. (1998) with a separate jet region that produces the non-thermal gamma-ray emission, and which explains the state transitions. Such a scenario will be discussed in the context of the observational evidence, summarized above, from the database produced by EBOP, JPL's BATSE earth occultation analysis system.

black holes↗

NASA NTRS1979

High-energy X-ray spectra of Cygnus XR-1 observed from OSO 8

X-ray spectra of Cygnus XR-1 were measured with the scintillation spectrometer aboard the OSO 8 satellite during a period of one-and-one-half to three weeks in each of the years from 1975 to 1977. Typical spectra of the source between 15 and 250 keV are presented and the spectra are found to be well represented by a single power-law expression whose photon number spectral index is different for the two intensity states that were considered. The observed pivoting effect is consistent with two-temperature accretion disk models of the X-ray emitting region.

Dolan, J. F.↗

NASA NTRS1983

Pair Production and Annihilation in Strong Magnetic Fields

Electromagnetic phenomena occurring in the presence of strong magnetic fields are currently of great interest in high-energy astrophysics. In particular, the process of pair production by single photons in the presence of fields of order 10 to the 12th power Gauss is of importance in cascade models of pulsar gamma ray emission, and may also become significant in theories of other radiation phenomena whose sources may be neutron stars (e.g., gamma ray bursts). In addition to pair production, the inverse process of pair annihilation is greatly affected by the presence of superstrong magnetic fields. The most significant departures from annihilation processes in free space are a reduction in the total rate for annihilation into two photons, a broadening of the familiar 511-keV line for annihilation at rest, and the possibility for annihilation into a single photon (which dominates the two-photon annihilation for B ( 10 the 13th power Gauss). The physics of these pair conversion processes, which is reviewed briefly, can become quite complex in the teragauss regime, and can involve calculations which are technically difficult to incorporate into models of emission mechanisms in neutron star magnetospheres. However, theoretical work, especially the case of pair annihilation, also suggests potential techniques for more direct measurements of field strengths near the stellar surface.

Daugherty, J. K.↗

NASA NTRS1983

Pair production and annihilation in strong magnetic fields

Electromagnetic phenomena occurring in the presence of strong magnetic fields are currently of great interest in high-energy astrophysics. In particular, the process of pair production by single photons in the presence of fields of order 10 to the 12th power Gauss is of importance in cascade models of pulsar gamma ray emission, and may also become significant in theories of other radiation phenomena whose sources may be neutron stars (e.g., gamma ray bursts). In addition to pair production, the inverse process of pair annihilation is greatly affected by the presence of superstrong magnetic fields. The most significant departures from annihilation processes in free space are a reduction in the total rate for annihilation into two photons, a broadening of the familiar 511-keV line for annihilation at rest, and the possibility for annihilation into a single photon which dominates the two-photon annihilation for B (10 to 13th power Gauss) The physics of these pair conversion processes, which is reviewed briefly, can become quite complex in the teragauss regime, and can involve calculations which are technically difficult to incorporate into models of emission mechanisms in neutron star magnetospheres. However, theoretical work, especially the case of pair annihilation, also suggests potential techniques for more direct measurements of field strengths near the stellar surface.

Daugherty, J. K.↗

DOE OSTI2024

Cherenkov photon background for low-noise silicon detectors in space

Future space observatories dedicated to direct imaging and spectroscopy of extra-solar planets will require ultra-low-noise detectors that are sensitive over a broad range of wavelengths. Silicon charge-coupled devices (CCDs), such as EMCCDs, Skipper CCDs, and Multi-Amplifier Sensing CCDs, have demonstrated the ability to detect and measure single photons from ultra-violet to near-infrared wavelengths, making them candidate technologies for this application. In this context, we study a relatively unexplored source of low-energy background coming from Cherenkov radiation produced by energetic charged particles traversing a silicon detector. In the intense radiation environment of space, energetic cosmic rays produce high-energy tracks and more extended halos of low-energy Cherenkov photons, which are detectable with ultra-low-noise detectors. We present a model of this effect that is calibrated to laboratory data, and we use this model to characterize the residual background rate for ultra-low noise silicon detectors in space. We find that the rate of cosmic-ray-induced Cherenkov photon production is comparable to other detector and astrophysical backgrounds that have previously been considered.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS2009

Quantum-Well Thermophotovoltaic Cells

Thermophotovoltaic cells containing multiple quantum wells have been invented as improved means of conversion of thermal to electrical energy. The semiconductor bandgaps of the quantum wells can be tailored to be narrower than those of prior thermophotovoltaic cells, thereby enabling the cells to convert energy from longer-wavelength photons that dominate the infrared-rich spectra of typical thermal sources with which these cells would be used. Moreover, in comparison with a conventional single-junction thermophotovoltaic cell, a cell containing multiple narrow-bandgap quantum wells according to the invention can convert energy from a wider range of wavelengths. Hence, the invention increases the achievable thermal-to-electrical energy-conversion efficiency. These thermophotovoltaic cells are expected to be especially useful for extracting electrical energy from combustion, waste-heat, and nuclear sources having temperatures in the approximate range from 1,000 to 1,500 C.

Freudlich, Alex↗

DOE OSTI2020

Quantum Hamiltonian for the surface charge density on a ring torus and radiative decay of plasmons

Photon scattering and the ensuing excitation of surface plasmons in single rings, single composite rings, and many-ring systems was recently shown to provide dispersion and field distributions [K. V. Garapati et al., J. Phys. Commun. 2, 015031 (2018)] of potential for specific applications in particle and molecular trapping [R. Alaee et al., Appl. Phys. Lett. 109, 141102 (2016); M. Salhi et al., Phys. Rev. A 92, 033416 (2015)], in addition to metamaterials and sensing. Furthermore, following photon or electron interactions with metallic nanorings, both radiative and nonradiative decay channels are important in the consideration of the nanoparticle as a photon or phonon source, and in related applications. In this work, we quantize the electronic normal modes of the ring torus and obtain the radiative decay of plasmons. Due to a geometry-related complexity, we employ a perturbation approach to obtain analytical expressions for the radiative decay channel for a vacuum bounded single solid nanoring. In quantizing the fields, the frequency spectrum of the charge density normal modes of the nanoring is obtained and shown to agree with the exact quasistatic plasmon dispersion relations. Higher-order corrections beyond the presented zero- and first-order calculations may be obtained following the presented results. The results are of potential interest in quantum sensing such as entangling photons and plasmons, or plasmons and trapped molecules.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗