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At least 1,063 records · Page 59

Correlated quadratures of resonance fluorescence and the generalized uncertainty relation

Resonance fluorescence from a two-state atom has been predicted to exhibit quadrature squeezing below the Heisenberg uncertainty limit, provided that the optical parameters (Rabi frequency, detuning, laser linewidth, etc.) are chosen carefully. When the correlation between two quadratures of the radiation field does not vanish, however, the Heisenberg limit for quantum fluctuations might be an unrealistic lower bound. A generalized uncertainty relation, due to Schroedinger, takes into account the possible correlation between the quadrature components of the radiation, and it suggests a modified definition of squeezing. We show that the coherence between the two levels of a laser-driven atom is responsible for the correlation between the quadrature components of the emitted fluorescence, and that the Schrodinger uncertainty limit increases monotonically with the coherence. On the other hand, the fluctuations in the quadrature field diminish with an increasing coherence, and can disappear completely when the coherence reaches 1/2, provided that certain phase relations hold.

Arnoldus, Henk F.↗

Decoding the Atomic Structure of Ga 2 Te 5 Pulsed Laser Deposition Films for Memory Applications Using Diffraction and First-Principles Simulations

Neuromorphic computing, reconfigurable optical metamaterials that are operational over a wide spectral range, holographic and nonvolatile displays of extremely high resolution, integrated smart photonics, and many other applications need next-generation phase-change materials (PCMs) with better energy efficiency and wider temperature and spectral ranges to increase reliability compared to current flagship PCMs, such as Ge 2 Sb 2 Te 5 or doped Sb 2 Te. Gallium tellurides are favorable compounds to achieve the necessary requirements because of their higher melting and crystallization temperatures, combined with low switching power and fast switching rate. Ga 2 Te 3 and non-stoichiometric alloys appear to be atypical PCMs; they are characterized by regular tetrahedral structures and the absence of metavalent bonding. The sp 3 gallium hybridization in cubic and amorphous Ga 2 Te 3 is also different from conventional p-bonding in flagship PCMs, raising questions about its phase-change mechanism. Furthermore, gallium tellurides exhibit a number of unexpected and highly unusual phenomena, such as nanotectonic compression and viscosity anomalies just above their melting points. Using high-energy X-ray diffraction, supported by first-principles simulations, we will elucidate the atomic structure of amorphous Ga 2 Te 5 PLD films, compare it with the crystal structure of tetragonal gallium pentatelluride, and investigate the electrical, optical, and thermal properties of these two materials to assess their potential for memory applications, among others.

36 MATERIALS SCIENCE↗

High-Purity Quantum Emission from an Au 24 (S-CH 2 Ph- t Bu) 20 Nanocluster at Room Temperature

Atomically precise gold nanoclusters have garnered significant attention for their diverse applications, ranging from biological labeling to optoelectronics. Their potential in optical quantum computing, which calls for ideal single-photon sources, has recently become a key area of interest. In the current work, we use photon antibunching experiments to explore the single-photon emission efficiency of atomically precise Au 24 nanoclusters protected by 4-tert-butylbenzyl mercaptan ligands (Au 24 (TBBM) 20 ). This cluster exhibits quantum emission with good photostability and without any observable blinking or spectral drift at room temperature under an inert gas atmosphere, with antibunching dips (g 2 (0)) as low as 0.07 in the solid state or, equivalently, a single-photon purity of 93% under time-gated conditions. Transient absorption and time-gated antibunching studies reveal that the short emission lifetime of this cluster and its high photoluminescence quantum yield in the solid state play critical roles in enhancing the emitted single-photon purity. This research advances the understanding of single-emitter behavior in atomically precise gold nanoclusters, contributing to the development of stable quantum emitters that are essential for quantum computing and cryptography.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Atomic-scale imaging of frequency-dependent phonon anisotropy

Directly visualizing vibrational anisotropy in individual phonon modes is essential for understanding a wide range of intriguing optical, thermal and elastic phenomena in materials. Although conventional optical and diffraction techniques have been used to estimate vibrational anisotropies, they fall short in achieving the spatial and energy resolution necessary to provide detailed information. Here, we introduce a new form of momentum-selective electron energy-loss spectroscopy, which enables the element-resolved imaging of frequency- and symmetry-dependent vibrational anisotropies with atomic resolution. Vibrational anisotropies manifest in different norms of orthogonal atomic displacements, known as thermal ellipsoids. Using the centrosymmetric strontium titanate as a model system, we observed two distinct types of oxygen vibrations with contrasting anisotropies: oblate thermal ellipsoids below 60 meV and prolate ones above 60 meV. In non-centrosymmetric barium titanate, our approach can detect subtle distortions of the oxygen octahedra by observing the unexpected modulation of q-selective signals between apical and equatorial oxygen sites near 55 meV, which originates from reduced crystal symmetry and may also be linked to ferroelectric polarization. These observations are quantitatively supported by theoretical modelling, which demonstrates the reliability of our approach. The measured frequency-dependent vibrational anisotropies shed new light on the dielectric and thermal behaviours governed by acoustic and optical phonons. Furthermore, the ability to visualize phonon eigenvectors at specific crystallographic sites with unprecedented spatial and energy resolution opens new avenues for exploring dielectric, optical, thermal and superconducting properties.

Ferroelectrics and multiferroics↗

Effect of Ram and Zenith Exposure on the Optical Properties of Polymers in Space

The temperature of spacecraft is influenced by the solar absorptance and thermal emittance of the external spacecraft materials. Optical and thermal properties can degrade over time in the harsh low Earth orbital (LEO) space environment where spacecraft external materials are exposed to various forms of radiation, thermal cycling, and atomic oxygen. Therefore, it is important to test the durability of spacecraft materials in the space environment. One objective of the Polymers and Zenith Polymers Experiments was to determine the effect of LEO space exposure on the optical properties of various spacecraft polymers. These experiments were flown as part of the Materials International Space Station Experiment 7 (MISSE 7) mission on the exterior of the International Space Station (ISS) for 1.5 years. Samples were flown in ram, wake or zenith directions, receiving varying amounts of atomic oxygen and solar radiation exposure. Total and diffuse reflectance and transmittance of flight and corresponding control samples were obtained post-flight using a Cary 5000 UV-Vis-NIR Spectrophotometer. Integrated air mass zero solar absorptance (s) of the flight and control samples were computed from the total transmittance and reflectance, and compared. The optical data are compared with similar polymers exposed to space for four years as part of MISSE 2, and with atomic oxygen erosion data, to help understand the degradation of these polymers in the space environment. Results show that prolonged space exposure increases the solar absorptance of some materials. Knowing which polymers remain stable will benefit future spacecraft design.

Yuanchun Li↗

Charge state dynamics and optically detected electron spin resonance contrast of shallow nitrogen-vacancy centers in diamond

Nitrogen-vacancy (NV) centers in diamond can be used for nanoscale sensing with atomic resolution and sensitivity; however, it has been observed that their properties degrade as they approach the diamond surface. Here we report that in addition to degraded spin coherence, NV centers within nanometers of the surface can also exhibit decreased fluorescence contrast for optically detected electron spin resonance (OD-ESR). We demonstrate that this decreased OD-ESR contrast arises from charge state dynamics of the NV center, and that it is strongly surface-dependent, indicating that surface engineering will be critical for nanoscale sensing applications based on color centers in diamond.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

In Situ Identification of Mineral Resources with an X-Ray-Optical "Hands-Lens" Instrument

The recognition of material resources on a planetary surface requires exploration strategies not dissimilar to those employed by early field geologists who searched for ore deposits primarily from surface clues. In order to determine the location of mineral ores or other materials, it will be necessary to characterize host terranes at regional or subregional scales. This requires geographically broad surveys in which statistically significant numbers of samples are rapidly scanned from a roving platform. To enable broad-scale, yet power-conservative planetary-surface exploration, we are developing an instrument that combines x-ray diffractometry (XRD), x-ray fluorescence spectrometry (XRF), and optical capabilities; the instrument can be deployed at the end of a rover's robotic arm, without the need for sample capture or preparation. The instrument provides XRD data for identification of mineral species and lithological types; diffractometry of minerals is conducted by ascertaining the characteristic lattice parameters or "d-spacings" of mineral compounds. D-spacings of 1.4 to 25 angstroms can be determined to include the large molecular structures of hydrated minerals such as clays. The XRF data will identify elements ranging from carbon (Atomic Number = 6) to elements as heavy as barium (Atomic Number = 56). While a sample is being x-rayed, the instrument simultaneously acquires an optical image of the sample surface at magnifications from lx to at least 50x (200x being feasible, depending on the sample surface). We believe that imaging the sample is extremely important as corroborative sample-identification data (the need for this capability having been illustrated by the experience of the Pathfinder rover). Very few geologists would rely on instrument data for sample identification without having seen the sample. Visual inspection provides critical recognition data such as texture, crystallinity, granularity, porosity, vesicularity, color, lustre, opacity, and so forth. These data can immediately distinguish sedimentary from igneous rocks, for example, and can thus eliminate geochemical or mineral ambiguities arising, say between arkose and granite. It would be important to know if the clay being analyzed was part of a uniform varve deposit laid down in a quiescent lake, or the matrix of a megabreccia diamictite deposited as a catastrophic impact ejecta blanket. The unique design of the instrument, which combines Debye-Scherrer geometry with elements of standard goniometry, negates the need for sample preparation of any kind, and thus negates the need for power-hungry and mechanically-complex sampling systems that would have to chip, crush, sieve, and mount the sample for x-ray analysis. Instead, the instrument is simply rested on the sample surface of interest (like a hand lens); the device can interrogate rough rock surfaces, coarse granular material, or fine rock flour. A breadboard version of the instrument has been deployed from the robotic arm of the Marsokhod rover in field trials at NASA Ames, where large vesicular boulders were x-rayed to demonstrate the functionality of the instrument design, and the ability of such a device to comply with constraints imposed by a roving platform. Currently under development is a flight prototype concept of this instrument that will weigh 0.3 kg, using about 4500 J of energy per sample analysis. It requires about 5 min. for XRD analysis, and about 30 min. for XRF interrogation. Its small mass and rugged design make it ideal for deployment on small rovers of the type currently envisaged for the exploration of Mars (e.g., Sojourner-scale platforms). The design utilizes a monolithic P-N junction photodiode pixel array for XRD, a Si PIN photodiode/avalanche photodiode system for XRF, and an endoscopic imaging camera system unobtrusively embedded between the detectors and the x-ray source (the endoscope with its board-mounted camera can be adapted for IR light in addition to visible wavelenths. A rugged, miniature (7 cu cm) x-ray source for the instrument has already been breadboarded.

Marshall, J.↗

All-aluminum optical system for a large cryogenically cooled far infrared echelle spectrometer

In the past few years, NASA's Kuiper Airborne Observatory (KAO) has made it possible to conduct pioneering observations of far infrared lines from astronomical sources. Such observations, in the case of wavelengths in the approximate range from 20 to 350 microns, cannot be performed from ground-based sites, because of telluric water absorption effects. Lines in the considered range provide information about the interstellar gas in molecular, neutral atomic, and ionized form of occurrence. The present paper provides a description of the development of the cryogenic optical system of a spectrometer designed to exploit the potential of the KAO for observing the far infrared lines. Attention is given to design goals and considerations, details of optical design, the fabrication of the optical system, the cryostat, and performance.

Erickson, E. F.↗

Isotope Shifts of Radium Monofluoride Molecules

Isotope shifts of 223–226,228 Ra 19 F were measured for different vibrational levels in the electronic transition A 2 II 1/2 ←X 2 Σ + . The observed isotope shifts demonstrate the particularly high sensitivity of radium monofluoride to nuclear size effects, offering a stringent test of models describing the electronic density within the radium nucleus. Ab initio quantum chemical calculations are in excellent agreement with experimental observations. These results highlight some of the unique opportunities that short-lived molecules could offer in nuclear structure and in fundamental symmetry studies.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The ultraviolet dayglow. IV - The spectrum and excitation of singly ionized oxygen

The emission line spectrum of singly ionized atomic oxygen (O II) dominates the day airglow spectrum in the extreme ultraviolet below 834 A. The strongest resonance line, at 834 A, is optically thick and an analysis of height profiles obtained from rocket observations between 140 and 265 km in specific viewing directions indicates that the principal excitation source is direct photoionization of neutral atomic oxygen. Strong emission at 538-539 A is most likely due to the quartet rather than the doublet transitions, which both occur at these wavelengths and which are not spectrally resolved in the data. The intensities of the weaker lines are consistent with recent laboratory measurements of transition branching ratios. Several strong O II lines near He I 584 produce severe contamination of low-altitude (less than 400 km) measurements of geocoronal helium emission made with thin-film broadband photometers.

Feldman, P. D.↗

SIREN: Scaling Ion-Traps by REquiring iNnovative Heterogenous Integration

The SIREN (Scaling Ion Traps by Requiring iNnovative heterogenous integration) project explores the feasibility of heterogeneous integration (HI) as a transformative approach to scaling ion traps, a critical technology for advancing quantum computers and atomic clocks. Traditional ion trap architectures face significant challenges in scalability due to limitations in optical access, fabrication techniques, and material constraints. SIREN addresses these challenges by leveraging HI, which combines different materials and fabrication processes to create more complex and efficient ion trap structures. HI integrated structures can be manufactured without compromising the process to maintain compatibility to ion traps. This project focuses on integrating a separately fabricated waveguide with a fully functional ion trap. The respective alignment between the pieces needs to be accurate to less than 2 µm to ensure that the light from the waveguide can overlap with the trapping region. The fine alignment must also be maintained through an ultra-high vacuum bake, a critical step in preparing an ion trap experiment. The project's outcomes suggest that heterogeneous integration is a promising pathway for overcoming current scalability barriers, paving the way for the next generation of quantum technologies. SIREN's findings contribute significantly to the field, offering a scalable solution that could accelerate the development of practical quantum computers and highly accurate atomic clocks.

42 ENGINEERING↗

Enantioselective Se lattices for stable chiroptoelectronic processing media

Chiroptoelectronic devices are crucial for applications in quantum computing, spin optical communications, and magnetic recording. However, the limited efficiency and low stability of conventional circularly polarized light (CPL)-sensing materials have restricted their broader use. Here, we introduce atomic chiral Se nanorod (NRs) films as broadband CPL detectors, leveraging the intrinsic chirality and stability of Se nanocrystals. We also perform incident circular polarization (ICP)-Raman optical activity (ROA) to explore the chiroptical activity of the large-area films. The Se NRs thin films detected CPL across a broad range from ultraviolet (UV) to short-wavelength infrared (SWIR), with a responsivity dissymmetry factor of up to 0.4, maintaining high stability under ambient conditions for longer than 13 months. CPL-sensitive Se NRs with intrinsic chirality have potential applications in chiral photonic synapses, chiral spin devices, and CPL-sensitive photocatalysts. ICP-ROA mapping also advances the analysis of 2D chiral materials.

Nanophotonics and plasmonics↗

Low-loss low thermo-optic coefficient Ta 2 O 5 on crystal quartz planar optical waveguides

Optical resonator-based frequency stabilization plays a critical role in ultra-low linewidth laser emission and precision sensing, atom clocks, and quantum applications. However, there has been limited success in translating traditional bench-top stabilization cavities to compact on-chip integrated waveguide structures that are compatible with photonic integration. The challenge lies in realizing waveguides that not only deliver low optical loss but also exhibit a low thermo-optic coefficient and frequency noise stability. Given the problematic sources of frequency noise within dielectrics, such as thermorefractive noise, resonators with small thermo-optic response are desirable for on-chip reference cavities. We report the first demonstration of a Ta 2 O 5 (tantala) waveguide core fabricated on a crystal quartz substrate lower cladding with TEOS-PECVD SiO 2 upper cladding. This waveguide offers significant advantages over other waveguides in terms of its low thermo-optic coefficient and reduced thermorefractive-related frequency noise. We describe the waveguide structure and key design parameters as well as fabrication considerations for processing tantala on quartz waveguides. We report a waveguide thermo-optic coefficient of -1.14 × 10 -6 RIU/K, a value that is over 6 times smaller in magnitude than that of SiO 2 -substrate tantala waveguides, with a propagation loss of 1.19 dB/cm at 1550 nm and <1.33 dB/cm across the 1525 nm–1610 nm wavelength range. Within a 1.6 mm radius ring resonator, we demonstrate a 2.54 × 10 5 intrinsic Q factor. With the potential for very low loss and the ability to control the thermal response, this waveguide platform takes a key step toward creating thermally stable integrated resonators for on-chip laser frequency stabilization and other applications.

42 ENGINEERING↗

Bias and uncertainty in the absorption emission measurement of atomic sodium density in the SSME exit plane

The measurement of atomic sodium concentration in the TTB 019 firing of April 1990 is significant in that it represents the first measurement of density at the exit plane of the space shuttle main engine. The knowledge of the sodium density, combined with the certainty that the exit plane of the plume is optically thin at the sodium D-line wavelengths, provides essential information for evaluation of diagnostic techniques using sodium atoms, such as resonant Doppler velocimetry for temperature, pressure, and velocity through high resolution fluorescent lineshape analysis. The technique used for the sodium atom line transmission (SALT) measurements is that of resonant absorption emission using a hollow cathode lamp as the reference source. Through the use of two-dimensional kinetic (TDK) predictions of temperature and density for the flight engine case and radiative transfer calculations, this line-of-sight spectrally integrated transmission indicates a sodium atom concentration, i.e., mole fraction, of 0.91e-10. The subject of this paper is the assumptions and measurement uncertainties tied into the calculation. Because of the narrow shape of the source emission, the uncertainties in the absorption profile could introduce considerable bias in the measurement. The following were investigated: (1) the inclusion of hyperfine splitting of the D-lines in the calculation; (2) the use of the flight engine predictions of plume temperature and density versus those for the large throat engine; (3) the assumption of a Gaussian, i.e., Doppler, distribution for the source radiance with a temperature of 400 K; (4) the use of atomic collisional shift and width values for the work by Jongerius; and (5) a Doppler shift for a 7 degree outward velocity vector at the plume edge. Also included in the study was the bias introduced by an uncertainty in the measurement of the D1/D2 line ratio in the source.

Bauman, Leslie E.↗

Optical Tweezers Array and Nimble Tweezers Probe Generated by Spatial- Light Modulator

An optical tweezers is being developed at the NASA Glenn Research Center as a visiblelight interface between ubiquitous laser technologies and the interrogation, visualization, manufacture, control, and energization of nanostructures such as silicon carbide (SiC) nanotubes. The tweezers uses one or more focused laser beams to hold micrometer-sized particles called tools (sometimes called tips in atomic-force-microscope terminology). A strongly focused laser beam has an associated light-pressure gradient that is strong enough to pull small particles to the focus, in spite of the oppositely directed scattering force; "optical tweezers" is the common term for this effect. The objective is to use the tools to create carefully shaped secondary traps to hold and assemble nanostructures that may contain from tens to hundreds of atoms. The interaction between a tool and the nanostructures is to be monitored optically as is done with scanning probe microscopes. One of the initial efforts has been to create, shape, and control multiple tweezers beams. To this end, a programmable spatial-light modulator (SLM) has been used to modify the phase of a laser beam at up to 480 by 480 points. One program creates multiple, independently controllable tweezer beams whose shapes can be tailored by making the SLM an adaptive mirror in an interferometer (ref. 1). The beams leave the SLM at different angles, and an optical Fourier transform maps these beams to different positions in the focal plane of a microscope objective. The following figure shows two arrays of multiple beams created in this manner. The patterns displayed above the beam array control the intensity-to-phase transformation required in programming the SLM. Three of the seven beams displayed can be used as independently controllable beams.

Decker, Arthur J.↗

Products of Dissociative Recombination in the Ionosphere

SRI International undertook a novel experimental measurement of the product states formed by dissociative recombination (DR) of O2(+), NO(+), and N2(+) as a function of both electron energy and reactant ion vibrational level. For these measurements we used a recently developed experimental technique for measuring dissociation product distributions that allows both the branching ratios to be accurately determined and the electronic and rovibrational state composition of the reactant ions to be specified. DR is the dominant electron loss mechanism in all regions of the ionosphere. In this process, electron attachment to the molecular ion produces an unstable neutral molecule that rapidly dissociates. For a molecular ion such as O2(+), the dissociation recombination reaction is (1) O2(+) + e yields O + O + W. The atomic products of this reaction, in this case two oxygen atoms, can be produced in a variety of excited states and with a variety of kinetic energies, as represented by W in Eq. (1). These atoms are not only active in the neutral chemistry of the ionosphere, but are also especially important because their optical emissions are often used to infer in situ concentrations of the parent molecular ion and ambient electron densities. Many laboratory measurements have been made of DR reaction rates under a wide range of electron temperatures, but very little is known about the actual distributions among the final states of the atomic products. This lack of knowledge seriously limits the validity and effectiveness of efforts to model both natural and man-made ionospheric disturbances. Bates recently identified major deficiencies in the currently accepted branching ratios for O2(+) as they relate to blue and green line emission measurements in the nocturnal F-region. During our two-year effort, we partially satisfied our ambitious goals. We constructed and operated a variable pressure, electron-impact ion source and a high pressure, hollow-cathode discharge ion source for O2(+), NO(+), and N2(+) beams. Translational spectroscopy of the products of dissociative charge transfer in Cs vapor was used to accurately assay the composition of the O2(+) and NO(+) beams and to develop a methodology for the vibrationally controlled preparation of the ground state ion beams. Attempts to assay the N2(+) beam revealed a novel two-electron process in the charge transfer reactions. A coaxial electron gun for the DR measurements was constructed following an extensive numerical design of the fields. Tests of the gun, however, found substantial perturbations of the magnetic fields by the soft iron (CMI-C) assembly containing the Langmuir probe that locates the electron beam. Hydrogen annealing of the iron failed to eliminate the field perturbations, necessitating the removal of the probe assembly. During this work on the coaxial electron gun, we discovered that predissociated high Rydberg states of O2 could be produced by subjecting the molecules to a sudden perturbation by an electromagnetic field. This technique allowed a measurement of the product branching to the atomic limits for the lowest seven vibrational levels of O2(+).

Cosby, Philip↗

Photonics Breakthroughs 2024: Narrow-Linewidth Lasers in the Visible and Near-Infrared

Narrow-linewidth lasers enable a variety of high-precision applications, such as sensing, optical clocks, and microwave frequency generation. Advances in photonic integration in the last decade led to the development of ultra-low-noise integrated semiconductor lasers, mostly in the telecom wavelength range. In recent years, the demand for high-performance lasers at shorter wavelengths skyrocketed, driven by applications in sensing and atom trapping. Low-noise lasers are of particular importance in this spectral range, as they are essential for optical clocks. Here, we will review recent progress in narrow-linewidth lasers at shorter wavelengths, present results on a hybrid-integrated low-noise laser at 780 nm and discuss the perspectives and challenges of high-performance semiconductor lasers in the visible and near-infrared.

Prokoshin, Artem [King Abdullah University of Scie↗

Amorphous silicon carbide coatings for extreme ultraviolet optics

Amorphous silicon carbide films formed by sputtering techniques are shown to have high reflectance in the extreme ultraviolet spectral region. X-ray scattering verifies that the atomic arrangements in these films are amorphous, while Auger electron spectroscopy and Rutherford backscattering spectroscopy show that the films have composition close to stoichiometric SiC, although slightly C-rich, with low impurity levels. Reflectance vs incidence angle measurements from 24 to 1216 A were used to derive optical constants of this material, which are presented here. Additionally, the measured extreme ultraviolet efficiency of a diffraction grating overcoated with sputtered amorphous silicon carbide is presented, demonstrating the feasibility of using these films as coatings for EUV optics.

Kortright, J. B.↗