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At least 109 records · Page 6

Development of Single Photon Sources in GaN

The recent discovery of bright, room-temperature, single photon emitters in GaN leads to an appealing alternative to diamond best single photon emitters given the widespread use and technological maturity of III-nitrides for optoelectronics (e.g. blue LEDs, lasers) and high-speed, high-power electronics. This discovery opens the door to on-chip and on-demand single photon sources integrated with detectors and electronics. Currently, little is known about the underlying defect structure nor is there a sense of how such an emitter might be controllably created. A detailed understanding of the origin of the SPEs in GaN and a path to deterministically introduce them is required. In this project, we develop new experimental capabilities to then investigate single photon emission from GaN nanowires and both GAN and AlN wafers. We ion implant our wafers with the ion implanted with our focused ion beam nanoimplantation capabilities at Sandia, to go beyond typical broad beam implantation and create single photon emitting defects with nanometer precision. We've created light emitting sources using Li + and He + , but single photon emission has yet to be demonstrated. In parallel, we calculate the energy levels of defects and transition metal substitutions in GaN to gain a better understanding of the sources of single photon emission in GaN and AlN. The combined experimental and theoretical capabilities developed throughout this project will enable further investigation into the origins of single photon emission from defects in GaN, AlN, and other wide bandgap semiconductors.

36 MATERIALS SCIENCE↗

Erbium-Implanted WS 2 Flakes with Room-Temperature Photon Emission at Telecom Wavelengths

Optically addressable spin impurities in crystals along with device engineering provide an attractive route to realizing quantum technologies in the solid state, but reconciling disparate emitter and host material constraints for a given target application is often challenging. Rare-earth ions in two-dimensional (2D) materials could mitigate this problem given the atomic-like transitions of the emitters and the versatile nature of van der Waals systems. Here we combine ion implantation, confocal microscopy, and ab initio calculations to examine the photon emission of Er-doped WS 2 flakes. Optical spectroscopy reveals narrow, long-lived photoluminescence lines in the telecom band, which we activate after low-temperature thermal annealing. Spectroscopic and polarization-selective measurements show a uniform response across the ensemble, while the fluorescence brightness remains mostly unchanged with temperature, suggesting nonradiative relaxation channels are inefficient. Our results create opportunities for novel solid state devices coupling 2D-hosted, telecom-band emitters to photonic heterostructures separately optimized for photon manipulation.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Tin–Lead Liquid Metal Alloy Source for Focused Ion Beams

Focused Ion Beam (FIB) systems are increasingly utilized in nanotechnology for nanostructuring, surface modification, doping, and rapid prototyping. Recently, their potential for quantum applications has been explored, leveraging FIB’s direct-write capabilities for in situ single ion implantation, which is crucial for fabricating single photon emitters. Color centers in diamond can function as qubits and are of particular interest due to their capacity to store and transmit quantum information. While Group-IV color centers exhibit high brightness, they require low temperatures to retain coherence. However, lead-vacancy in diamond (PbV) operates at the higher end (4 K) of this temperature spectrum due to larger ground-state splitting, making them particularly interesting. In this context, our study presents results for lead (Pb)-containing alloys with eutectic points below 600 °C and results on using tantalum (Ta) and titanium (Ti) as emitter materials for a Pb liquid metal alloy ion source. We show that a standard FIB system is able to resolve the different Pb isotopes and achieve nanoscale spot sizes, as required for quantum information science applications.

color center↗

Room-temperature high-purity single-photon emission from carbon-doped boron nitride thin films

Hexagonal boron nitride (h-BN) has emerged as a promising platform for generating room temperature single photons exhibiting high brightness and spin-photon entanglement. However, improving emitter purity, stability, and scalability remains a challenge for quantum technologies. Here, we demonstrate highly pure and stable single-photon emitters (SPEs) in h-BN by directly growing carbon-doped, centimeter-scale h-BN thin films using the pulsed laser deposition (PLD) method. These SPEs exhibit room temperature operation with polarized emission, achieving a g (2) (0) value of 0.015, which is among the lowest reported for room temperature SPEs and the lowest achieved for h-BN SPEs. It also exhibits high brightness (~0.5 million counts per second), remarkable stability during continuous operation (>15 min), and a Debye-Waller factor of 45%. First-principles calculations reveal unique carbon defects responsible for these properties, enabled by PLD’s low-temperature synthesis and in situ doping. Our results demonstrate an effective method for large-scale production of high-purity, stable SPEs in h-BN, enabling robust quantum optical sources for various quantum applications.

36 MATERIALS SCIENCE↗

Band Edge Excitons and Amplified Spontaneous Emission of Mercury Chalcogenide Nanoplatelets

Colloidal nanoplatelets of HgSe and HgTe prepared indirectly through cation exchange reactions can transfer many of the advantageous properties of atomically precise, 2D cadmium chalcogenides to the near-infrared (NIR) spectral window. In this work, HgSe and HgTe nanoplatelets are studied to understand their fundamental photophysical properties, particularly those areas of similarity and difference from cadmium-based NPLs, and to examine their potential as optical gain media. Similar to cadmium chalcogenide NPLs, low-temperature photoluminescence of HgTe NPLs displays two-color emission that depends on temperature, sample, fluence, excitation frequency, and irradiation time. Both HgTe and HgSe show nanosecond emission dynamics at temperatures as low as 2.5 K, with no indication that bright-dark excitonic splitting governs the low-temperature photoluminescence. Collectively, experimental data is most consistent with emission from a negative trion state at low temperature. Although the mercury chalcogenide nanoplatelets are shown to have broadened optical resonances compared to the cadmium chalcogenides from which they are derived, they retain slow Auger recombination and can display low-threshold amplified spontaneous emission in the NIR spectral window. Optical pumping thresholds for HgTe NPLs are observed as low as 4.4 µJ cm -2 and highlight the potential 2D nanoplatelets as gain medium in the near-infrared.

36 MATERIALS SCIENCE↗

The Rest-frame Submillimeter Spectrum of High-redshift, Dusty, Star-forming Galaxies from the SPT-SZ Survey

We present the average rest-frame spectrum of the final catalog of dusty star-forming galaxies (DSFGs) selected from the South Pole Telescope's SPT-SZ survey and measured with Band 3 of the Atacama Large Millimeter/submillimeter Array. This work builds on the previous average rest-frame spectrum, given in Spilker et al. (2014) for the first 22 sources, and is comprised of a total of 78 sources, normalized by their respective apparent dust masses. The spectrum spans 1.9 < z < 6.9 and covers rest-frame frequencies of 240–800 GHz. Combining this data with low-J CO observations from the Australia Telescope Compact Array, we detect multiple bright line features from 12 CO, [Ci], and H 2 O, as well as fainter molecular transitions from 13 CO, HCN, HCO + , HNC, CN, H 2 O + , and CH. We use these detections, along with limits from other molecules, to characterize the typical properties of the interstellar medium (ISM) for these high-redshift DSFGs. We are able to divide the large sample into subsets in order to explore how the average spectrum changes with various galaxy properties, such as effective dust temperature. We find that systems with hotter dust temperatures exhibit differences in the bright 12 CO emission lines, and contain either warmer and more excited dense gas tracers or larger dense gas reservoirs. These observations will serve as a reference point to studies of the ISM in distant luminous DSFGs (L IR > 10 12 L ⊙ ), and will inform studies of chemical evolution before the peak epoch of star formation at z = 2–3.

79 ASTRONOMY AND ASTROPHYSICS↗

Numerical characterization of quasi-steady thermal load for thin crystal at cryogenic temperature with nondiffusive heat transfer

With dramatically improved brightness and repetition rate, the thermal load for crystal optics in x-ray free-electron laser applications has also significantly increased. To mitigate the thermal load, one effective method is cryogenic cooling. However, the emerging nondiffusive heat transfer phenomenon at cryogenic temperature may cause design failure if overlooked. To evaluate the optical performance of thin crystal optics under thermal load at cryogenic temperature, an integrated numerical tool is presented and applied to characterize the thermal load on thin crystals with nondiffusive phenomena accounted. Significant thermally induced distortion of the rocking curve is observed from numerical simulation, leading to potential seed power reduction in hard x-ray self-seeding application. Cryogenic cooling is confirmed necessary by simulation to handle the thermal load at high repetition rate operation.

42 ENGINEERING↗

A hybrid coupler for directing quantum light emission with high radiative Purcell enhancement to a dielectric metasurface lens

Quantum photonic technologies such as quantum sensing, metrology, and simulation could be transformatively enabled by the availability of integrated single photon sources with high radiative rates and photon collection efficiencies. We address these challenges for quantum emitters formed from color center defect sites such as those in hexagonal boron nitride, which are promising candidates as single photon sources due to their bright, stable, polarized, and room temperature emission. We report design of a nanophotonic coupler from color center quantum emitters to a dielectric metasurface lens. The coupler is comprised of a hybrid plasmonic–dielectric resonator that achieves a large radiative Purcell enhancement and partial control of far-field radiation. We report radiative Purcell factors up to 285 and photon collection efficiencies up to 89% for a lossless metasurface, applying a continuous hyperboloidal phase-front. Our hybrid plasmonic–dielectric coupler interfacing two nanophotonic elements is a compound optical element, analogous to those found in microscope objective lenses, which combine multiple optical functions into a single component for improved performance.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Emissive Colloidal GaAs Quantum Dots

Colloidal quantum dots offer tunable optical properties for optoelectronic applications, but the synthesis of high-quality III–V quantum dots (QDs) other than indium pnictides, and particularly GaAs, has remained elusive due to synthetic challenges. Colloidal GaAs QDs have been reported very recently and have shown only weak band-edge photoluminescence. Here, we demonstrate a large-scale synthesis of colloidal GaAs QDs in molten salts, followed by a high-temperature surface treatment with K 2 S, which removes native oxide and enables uniform zinc chalcogenide shell growth on GaAs. These QDs demonstrate bright band-edge photoluminescence and electroluminescence in QD LED devices. Low-temperature spectroscopy reveals a well-resolved exciton fine structure with distinct bright-state splitting and temperature-independent decay dynamics from 4 to 100 K. These results establish a practical pathway for the preparation of high-quality colloidal GaAs QDs from molten salts with potential applications in quantum technologies and optoelectronics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Impact of in situ nuclear networks and atomic opacities on neutron star merger ejecta dynamics, nucleosynthesis, and kilonovae

Context. Binary neutron star merger (BNSM) ejecta are key sites of rapid neutron capture (r-process) nucleosynthesis and they produce kilonovae powered by the radioactive decay of freshly synthesized nuclei. Modeling their evolution requires multi-physics simulations involving hydrodynamics, nuclear reactions, and radiative processes. The impact of nuclear burning and atomic opacity is poorly understood and often treated with simplified prescriptions. Aims. We systematically investigate different treatments of nuclear heating, particle thermalization, and atomic opacities in radiation-hydrodynamics simulations of BNSM ejecta and kilonova light curves. Methods. Ejecta profiles from long-term numerical-relativity simulations of asymmetric neutron star binaries with a massive neutron star remnant were evolved to ∼30 days using a 2D ray-by-ray approach. We compared simplified heating-rate and thermalization prescriptions with in situ Nuclear reaction Network (NN) calculations that track nuclear energy deposition and include a composition-dependent thermalization scheme. We also contrasted various gray opacity models with a frequency-dependent treatment based on atomic calculations. Results. Coupling NN and hydrodynamics significantly affects nucleosynthesis and kilonova emission. Assuming homologous expansion alters abundance evolution and produces a narrower, less populated second r-process peak and a third peak shifted to higher mass numbers. The back-reaction of nuclear heating affects the temperature evolution enough to delay and redden the early (t∼ hours) kilonova peaks. A constant thermalization efficiency underestimates and reddens the early emission while overestimating the late-time luminosity compared to the composition-dependent treatment. Analytical opacity prescriptions yield a more extended, colder photosphere, resulting in dimmer, redder kilonovae at early times (t≲ hour), while the delayed recession of the photosphere prolongs the red emission at t ≳ 5 days. Conclusions. Coupling hydrodynamics to an in situ NN is crucial for reliable nucleosynthesis and kilonova predictions. Resolving the first several hundred milliseconds of the hydrodynamics is essential for robust nucleosynthesis calculations. Composition-dependent thermalization and frequency-dependent, atomic-physics-based opacities are needed to accurately capture the temperature evolution of the ejecta and the brightness and color evolution of the kilonova. Calibrated analytic nuclear-power fits with simplified thermalization and opacity prescriptions can still reproduce the density and temperature evolution of the ejecta.

74 ATOMIC AND MOLECULAR PHYSICS↗

Identification and demonstration of roGFP2 as an environmental sensor for cryogenic correlative light and electron microscopy

Cryogenic correlative light and electron microscopy (cryo-CLEM) seeks to leverage orthogonal information present in two powerful imaging modalities. While recent advances in cryogenic electron microscopy (cryo-EM) allow for the visualization and identification of structures within cells at the nanometer scale, information regarding the cellular environment, such as pH, membrane potential, ionic strength, etc., which influences the observed structures remains absent. Fluorescence microscopy can potentially be used to reveal this information when specific labels, known as fluorescent biosensors, are used, but there has been minimal use of such biosensors in cryo-CLEM to date. Here we demonstrate the applicability of one such biosensor, the fluorescent protein roGFP2, for cryo-CLEM experiments. At room temperature, the ratio of roGFP2 emission brightness when excited at 425 nm or 488 nm is known to report on the local redox potential. When samples containing roGFP2 are rapidly cooled to 77 K in a manner compatible with cryo-EM, the ratio of excitation peaks remains a faithful indicator of the redox potential at the time of freezing. Using purified protein in different oxidizing/reducing environments, we generate a calibration curve which can be used to analyze in situ measurements. As a proof-of-principle demonstration, we investigate the oxidation/reduction state within vitrified Caulobacter crescentus cells. The polar organizing protein Z (PopZ) localizes to the polar regions of C. crescentus where it is known to form a distinct microdomain. Finally, by expressing an inducible roGFP2-PopZ fusion we visualize individual microdomains in the context of their redox environment.

59 BASIC BIOLOGICAL SCIENCES↗

Improving Strain-localized GaSe Single Photon Emitters with Electrical Doping

Exciton localization through nanoscale strain has been used to create highly efficient single-photon emitters (SPEs) in 2D materials. However, the strong Coulomb interactions between excitons can lead to nonradiative recombination through exciton–exciton annihilation, negatively impacting SPE performance. Here, we investigate the effect of Coulomb interactions on the brightness, single photon purity, and operating temperatures of strain-localized GaSe SPEs by using electrostatic doping. By gating GaSe to the charge neutrality point, the exciton–exciton annihilation nonradiative pathway is suppressed, leading to ∼60% improvement of emission intensity and an enhancement of the single photon purity g (2) (0) from 0.55 to 0.28. The operating temperature also increased from 4.5 K to 85 K consequently. In conclusion, this research provides insight into many-body interactions in excitons confined by nanoscale strain and lays the groundwork for the optimization of SPEs for optoelectronics and quantum photonics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spectroscopic confirmation of a mature galaxy cluster at a redshift of 2

Galaxy clusters are the most massive virialized structures in the Universe and are formed through the gravitational accretion of matter over cosmic time. The discovery of an evolved galaxy cluster at redshift z = 2, corresponding to a look-back time of 10.4 billion years, provides an opportunity to study its properties. The galaxy cluster XLSSC 122 was originally detected as a faint, extended X-ray source in the XMM Large Scale Structure survey and was revealed to be coincident with a compact over-density of galaxies with photometric redshifts of 1.9 ± 0.2. Subsequent observations at millimetre wavelengths detected a Sunyaev–Zel’dovich decrement along the line of sight to XLSSC 122, thus confirming the existence of hot intracluster gas, while deep imaging spectroscopy from the European Space Agency’s X-ray Multi-Mirror Mission (XMM-Newton) revealed an extended, X-ray-bright gaseous atmosphere with a virial temperature of 60 million Kelvin, enriched with metals to the same extent as are local clusters. Here we report optical spectroscopic observations of XLSSC 122 and identify 37 member galaxies at a mean redshift of 1.98, corresponding to a look-back time of 10.4 billion years. We use photometry to determine a mean, dust-free stellar age of 2.98 billion years, indicating that star formation commenced in these galaxies at a mean redshift of 12, when the Universe was only 370 million years old. The full range of inferred formation redshifts, including the effects of dust, covers the interval from 7 to 13. These observations confirm that XLSSC 122 is a remarkably mature galaxy cluster with both evolved stellar populations in the member galaxies and a hot, metal-rich gas composing the intracluster medium.

79 ASTRONOMY AND ASTROPHYSICS↗

Observation of biexciton emission from single semiconductor nanoplatelets

Quasi-two-dimensional semiconductor nanoplatelets (NPLs) are intriguing systems for studying the influence of Auger recombination processes on the multiexciton emission efficiencies in the weak in-plane confinement regime. We investigate CdSe/CdS core/shell NPLs using cryogenic temperature single particle spectroscopy and observe bright biexciton emission at high excitation powers. The average binding energy of the biexcitons is determined to be 16.5 meV. The observed switching between the biexciton and trion states indicates charging-decharging dynamics of the NPLs mediated by the Auger ionization process. These findings are highly relevant for harvesting efficient biexciton emission for energy, lighting, and quantum applications.

36 MATERIALS SCIENCE↗

A cryogenically cooled 200 kV DC photoemission electron gun for ultralow emittance photocathodes

Novel photocathode materials like ordered surfaces of single crystal metals, epitaxially grown high quantum efficiency thin films, and topologically non-trivial materials with dirac cones show great promise for generating brighter electron beams for various accelerator and ultrafast electron scattering applications. Despite several materials being identified as brighter photocathodes, none of them have been tested in electron guns to extract electron beams due to technical and logistical challenges. In this paper, we present the design and commissioning of a cryocooled 200 kV DC electron gun that is capable of testing a wide variety of novel photocathode materials over a broad range of temperatures from 298 to 35 K for bright electron beam generation. This gun is designed to enable easy transfer of the photocathode to various standard ultra-high-vacuum surface diagnostics and preparation techniques, allowing a full characterization of the dependence of beam brightness on the photocathode material and surface properties. We demonstrate the development of such a high-voltage, high-gradient gun using materials and equipment that are easily available in any standard university lab, making the development of such 200 kV electron guns more accessible.

Instruments & Instrumentation↗

Dark-exciton energy splitting in monolayer W Se 2 : Insights from time-dependent density functional theory

Here, we present here a formalism based on time-dependent density functional theory to describe characteristics of both intra- and intervalley excitons in semiconductors, the latter of which had remained a challenge. Through the usage of an appropriate exchange-correlation kernel (nanoquanta), we trace the energy difference between the intra- and intervalley dark excitons in monolayer (1L) W⁢ Se 2 to the domination of the exchange part in the exchange-correlation energies of these states. Furthermore, our calculated transition contribution maps establish the momentum resolved weights of the electron-hole excitations in both bright and dark excitons thereby providing a comprehensive understanding of excitonic properties of 1L W⁢ Se 2 . We find that the states consist of hybridized excitations around the corresponding valleys which leads to brightening of the dark excitons, i.e., significantly decreasing their lifetime which is reflected in the PL spectrum. Using many-body perturbation theory, we calculate the phonon contribution to the energy band gap and the linewidths of the excited electrons, holes, and (bright) exciton to find that as the temperature increases the band gap significantly decreases, while the linewidths increase. Our work paves for describing the ultrafast charge dynamics of transition metal dichalcogenide within an ab initio framework.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Solution-Processed Ultrafast, Room-Temperature Single-Photon Source at 1550 nm

Single photons are cornerstones of quantum technologies. The need for an ultrafast, bright, and stable photon source emitting in the telecom-band at ∼1550 nm, ideally operating at room temperature, has resulted in a decades-long quest. However, to date, telecom sources are hampered by inherently long radiative lifetimes that severely limit brightness and speed, material instability, or the need for cryogenic operation. Here, in this study, stable colloidal PbS/CdS quantum dots emitting at 1550 nm (C-band) or 1350 nm (O-band) are embedded in a solution-synthesized nanoparticle-on-mirror cavity. Single cavity-coupled quantum dots experience extreme Purcell factors up to 10,700, resulting in ultrafast emission lifetimes of 65 ps, along with near-complete blinking suppression. As a result, 12 million single photons are emitted per second affording a single photon source at 1550 nm that is more than two orders of magnitude brighter than previously possible at room-temperature. These telecom-band single photon sources are solution-processable and lithography-free and may leverage mature colloidal fabrication technologies for future quantum applications.

36 MATERIALS SCIENCE↗