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NASA NTRS1980

Two-photon excitation cross section in light and intermediate atoms in frozen-core LS-coupling approximation

Using the method of explicit summation over the intermediate states two-photon absorption cross sections in light and intermediate atoms based on the simplistic frozen-core approximation and LS coupling have been formulated. Formulas for the cross section in terms of integrals over radial wave functions are given. Two selection rules, one exact and one approximate, valid within the stated approximations are derived. The formulas are applied to two-photon absorptions in nitrogen, oxygen, and chlorine. In evaluating the radial integrals, for low-lying levels, the Hartree-Fock wave functions, and for high-lying levels, hydrogenic wave functions obtained by the quantum-defect method have been used. A relationship between the cross section and the oscillator strengths is derived.

Omidvar, K.↗

DOE OSTI2025

An Integrated High-Speed Microstructural Characterization Method Using Simultaneous XRD, Stereo-DIC, and PCI

High-speed characterization of the deformation mechanisms in polycrystalline metals requires the quantification of full strain fields and local microstructural evolutions simultaneously. In this paper, we present a novel experimental method to integrate phase-contrast imaging (PCI), stereographic digital image correlation (stereo-DIC), and full-ring X-ray diffraction (XRD) to allow for the simultaneous characterization of polycrystalline metals at 1MHz or higher. A Kolsky bar was integrated into the synchrotron X-ray source in Sector 32 ID-B at the Advance Photon Source (APS) at Argonne National Laboratory. When the sample is dynamically loaded, the diagnostic methods of full-ring XRD, PCI, and stereo-DIC are properly synchronized to record the deformation behavior at both continuum and microstructural scales as a function of the loading history. An advanced high-strength steel (AHSS) is used as a model material to demonstrate the capabilities of this new experimental method.

36 MATERIALS SCIENCE↗

NASA NTRS2022

Constraints on Axions from Cosmic Distance Measurements

Axion couplings to photons could induce photon-axion conversion in the presence of magnetic fields in the Universe. This conversion could impact various cosmic distance measurements, such as luminosity distances to type Ia supernovae and angular distances to galaxy clusters, in different ways. In this paper we consider different combinations of the most up-to-date distance measurements to constrain the axion-photon coupling. Employing the conservative cell magnetic field model for the magnetic fields in the intergalactic medium (IGM) and ignoring the conversion in the intracluster medium (ICM), we find the upper bounds on axion-photon couplings to be around 5 × 10^(−12) (nG/B) √(Mpc/s) Ge/V for axion masses m(a) below 10^(−13) eV, where B is the strength of the IGM magnetic field, and s is the comoving size of the magnetic domains. When including the conversion in the ICM, the upper bound is lowered and could reach 5 × 10^(−13) Ge/V for m(a) < 5 × 10^(−12) eV. While this stronger bound depends on the ICM modeling, it is independent of the strength of the IGM magnetic field, for which there is no direct evidence yet. These constraints could be placed on firmer footing with an enhanced understanding and control of the astrophysical uncertainties associated with the IGM and ICM. All the bounds are determined by the shape of the Hubble rate as a function of redshift reconstructable from various distance measurements, and insensitive to today’s Hubble rate, of which there is a tension between early and late cosmological measurements. As an appendix, we discuss the model building challenges of the use of photon-axion conversion to make type Ia supernovae brighter to alleviate the Hubble problem/crisis.

Cosmology of Theories beyond the SM↗

DOE OSTI2025

Shell Thickness and Heterogeneity Dependence of Triplet Energy Transfer between Core–Shell Quantum Dots and Adsorbed Molecules

Quantum dot (QD)-sensitized triplet energy transfer (TET) has found promising applications in photon upconversion and photocatalysis. However, the underlying mechanism of TET in the QD-acceptor complex remains unclear despite the well-developed TET theory for the molecular donor–acceptor systems. Herein, the coupling strength of TET from CdSe/CdS core–shell QDs to 9-anthracene carboxylic acid (ACA) was studied by measuring the TET rate as a function of shell thickness with time-resolved photoluminescence. The change of TET-coupling strength with increasing shell thickness was further compared to those of electron and hole transfers from QDs so that we could test whether QD-sensitized TET is mediated by the charge transfer virtual state and can be considered as simultaneous electron and hole transfers as in molecular donor–acceptor systems. The measured coupling strength of TET from the CdSe/CdS QD decreases exponentially with the CdS shell thickness r: |V|(r) = |V|(0)e –βr , with an exponential decay factor β of 0.19 Å –1 , which is smaller than the sum of the measured decay factors for electron transfer to methyl viologen (0.18 Å –1 ) and hole transfer to phenothiazine (0.29 Å –1 ) from the same QD. This inconsistency is explained by the broadening of QD shell thicknesses in the distance dependence study, which significantly modifies the TET-coupling strength and driving force, resulting in a shallower distance dependence of the TET rate constants. This study sheds light on the fundamental mechanisms of QD-sensitized TET reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Ab initio evaluation of the electronic and optical properties of V B C B defect in wurtzite boron nitride as promising single-photon emitter

Single-photon emitters (SPEs) in the near-infrared (NIR) range with sharp and intense zero-phonon lines (ZPLs) of emission are critical for quantum communications. Certain local defects in wide-bandgap semiconductors create isolated occupied and unoccupied states within the bandgap of the host semiconductor and thus exhibit sharp ZPLs of emission. We designed and studied a defect in the wurtzite boron nitride as a potential SPE. It consists of a boron vacancy and a carbon atom substituting another boron atom (V B C B defect). The density of states is obtained within the GW method to identify favorable local defect states that may dominate optical transitions. The dielectric function and oscillator strength of the V B C B defect are obtained using the Bethe-Salpeter equation method to identify the optical excitations of the V B C B defect, from which we conclude that the defect could be a source of NIR emission with a narrow bright ZPL peak, thus an efficient SPE.

36 MATERIALS SCIENCE↗

DOE OSTI2021

High resolution >40 keV x-ray radiography using an edge-on micro-flag backlighter at NIF-ARC

Radiography of low-contrast features in high-density materials evolving on a nanosecond timescale requires a bright photon source in the tens of keV range with high temporal and spatial resolution. One application for sources in this category is the study of dynamic material strength in samples compressed to Mbar pressures at the National Ignition Facility, high-resolution measurements of plastic deformation under conditions relevant to meteor impacts, geophysics, armor development, and inertial confinement fusion. Here, we present radiographic data and the modulation transfer function (MTF) analysis of a multi-component test object probed at ~100 keV effective backlighter energy using a 5 μm-thin dysprosium foil driven by the NIF Advanced Radiographic Capability (ARC) short-pulse laser (~2 kJ, 10 ps). The thin edge of the foil acts as a bright line-projection source of hard x rays, which images the test object at 13.2× magnification into a filtered and shielded image plate detector stack. The system demonstrates a superior contrast of shallow (5 μm amplitude) sinusoidal ripples on gold samples up to 90 μm thick as well as enhanced spatial and temporal resolution using only a small fraction of the laser energy compared to an existing long-pulse-driven backlighter used routinely at the NIF for dynamic strength experiments.

47 OTHER INSTRUMENTATION↗

NASA NTRS1992

Synchrotron emission from a cosmological jet as a model of gamma-ray bursts

The nonthermal rapidly varying spectra of gamma-ray bursts require relativistic beaming if the source is at a cosmological distance. Limits on the Lorentz factors and magnetic fields of extragalactic jet models of gamma-ray bursts are derived from the synchrotron source function, the position of the fundamental cyclotron resonance, the Thomson optical depth of radiating electrons, and the Thomson optical depth of electron-positron pairs created in photon-photon collisions of Compton upscattered radiation. The last of these constraints is the strongest, and it is satisfied by the observations if the jet's Lorentz factor is greater than 100. The limit from the position of the cyclotron fundamental requires a magnetic field strength below approximately 10 exp 10 G. Jet models producing observable cyclotron lines are allowed. The acceleration region in the burst must be separate from the emission region. The similarity of gamma-ray burst jet models to models of quasars and BL Lac objects suggest that if gamma-ray bursts are cosmological sources, they are a type of active galaxy.

Brainerd, J. J.↗

NASA NTRS1992

Dynamic light scattering analysis of solutions from which lysozyme crystals grow

The variation of the friction factor was measured by photon correlation spectroscopy during isothermal growth of chicken egg white lysozyme crystals. It was observed to initially increase to a maximum as crystals formed, and then to decrease to a constant value. The change in the friction factors was measured as a function of temperature at concentrations of lysozyme varying from one sufficiently low that molecular interactions were undetectable to concentrations near those at which crystals grow in solutions, in all cases the ionic strength was below that required for crystallization.

Bishop, J. B.↗

DOE OSTI2021

Franck-Condon Tuning of Optical Cycling Centers by Organic Functionalization

Laser induced electronic excitations that spontaneously emit photons and decay directly to the initial ground state (“optical cycling transitions”) are used in quantum information and precision measurement for state initialization and readout. To extend this primarily atomic technique to large, organic compounds, we theoretically investigate optical cycling of alkaline earth phenoxides and their functionalized derivatives. We find that optical cycle leakage due to wave function mismatch is low in these species, and can be further suppressed by using chemical substitution to boost the electron-withdrawing strength of the aromatic molecular ligand through resonance and induction effects. This provides a straightforward way to use chemical functional groups to construct optical cycling moieties for laser cooling, state preparation, and quantum measurement.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1986

Compton scattering in strong magnetic fields

The relativistic cross section for Compton scattering by electrons in strong magnetic fields is derived. The results confirm and extend earlier work which has treated only transitions to the lowest or first excited Landau levels. For the teragauss field strengths expected in neutron star magnetospheres, the relative rates for excited state transitions are found to be significant, especially for incident photon energies several times the cyclotron frequency. Since these transitions must result in the rapid emission of one or more cyclotron photons as well as the Compton-scattered photon, the scattering process actually becomes a photon 'splitting' mechanism which acts to soften hard photon spectra, and also provides a specific mechanism for populating higher Landau levels in the electron distribution function. The results should be significant for models of gamma-ray bursters and pulsating X-ray sources.

Daugherty, Joseph K.↗

DOE OSTI2023

Measurement of $Z\gamma \gamma$ production in pp collisions at $\sqrt{s}= 13$ TeV with the ATLAS detector

Cross-sections for the production of a $Z$ boson in association with two photons are measured in proton–proton collisions at a centre-of-mass energy of 13 TeV. The data used correspond to an integrated luminosity of 139 fb -1 recorded by the ATLAS experiment during Run 2 of the LHC. The measurements use the electron and muon decay channels of the $Z$ boson, and a fiducial phase-space region where the photons are not radiated from the leptons. The integrated $Z$($\rightarrow$ $\ell$$\ell$)$\gamma \gamma$ cross-section is measured with a precision of 12% and differential cross-sections are measured as a function of six kinematic variables of the $Z\gamma \gamma$ system. The data are compared with predictions from MC event generators which are accurate to up to next-to-leading order in QCD. The cross-section measurements are used to set limits on the coupling strengths of dimension-8 operators in the framework of an effective field theory.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS2020

SNPP VIIRS RSB on-orbit radiometric calibration algorithms Version 2.0 and the performances. Part I: The algorithms

The first VIIRS instrument is aboard the Suomi National Polar-orbiting Partnership satellite. The instrument has 14 reflective solar bands (RSBs) to passively collect photons reflected from the Earth surface in the design wavelengths from 412 to 2250 nm. The instrument uses a solar diffuser (SD) to radiometrically calibrate its RSBs. When lit by the Sun through an attenuation screen (the SD screen), the SD diffusely reflects off the incident sunlight to act as a radiance source for the calibration. An onboard solar diffuser stability monitor (SDSM) yields the on-orbit change of the SD bidirectional reflectance distribution function (BRDF) by comparing the signal strength from the SD with that from the Sun attenuated by another attenuation screen (the SDSM screen). Complications arise due to the discovery that the on-orbit change of the BRDF is angle dependent. Additionally, the SDSM does not cover the wavelengths for the short-wave infrared bands in the RSBs. Furthermore, satellite yaw maneuvers were performed in the early mission to yield data for refining the prelaunch SDSM screen relative effective transmittance and the relative product of the SD screen transmittance and the BRDF at the mission start. But the yaw maneuver data are coarse in the solar azimuth angles and thus are unable to yield accurate values between the measurement angles. Over the years of performing on-orbit radiometric calibration through the SD for the VIIRSRSBs, we have developed several highly effective calibration algorithms to address the issues mentioned above. This paper reviews these algorithms.

on-orbit cailbration↗

NASA NTRS2020

SNPP VIIRS RSB on-orbit radiometric calibration algorithms Version 2.0 and the performances. Part I: The algorithms

Ning Lei↗

NASA NTRS1991

Magnetic two-photon scattering and two-photon emission - Cross sections and redistribution functions

The magnetic two-photon scattering cross section is discussed within the framework of QED, and the corresponding scattering redistribution function for this process and its inverse, as well as the scattering source function are calculated explicitly. In a similar way, the magnetic two-photon emission process which follows the radiative excitation of Landau levels above ground is calculated. The two-photon scattering and two-photon emission are of the same order as the single-photon magnetic scattering. All three of these processes, and in optically thick cases also their inverses, are included in radiative transport calculations modeling accreting pulsars and gamma-ray bursters. These processes play a prominent role in determining the relative strength of the first two cyclotron harmonics, and their effects extend also to the higher harmonics.

Alexander, S. G.↗

DOE OSTI2024

Symmetry Breaking in the Lowest-Lying Excited-State of CCl4: Valence Shell Spectroscopy in the 5.0–10.8 eV Photon Energy Range

We report absolute high-resolution vacuum ultraviolet (VUV) photoabsorption cross-sections of carbon tetrachloride (CCl4) in the photon energy range 5.0–10.8 eV (248–115 nm). The molecular spectrum and electronic structure have been comprehensively investigated together with quantum chemical calculations, providing geometries, bond lengths, vertical excitation energies and oscillator strengths. The major electronic excitations have been assigned to valence and Rydberg transitions which are also accompanied by vibrational excitation assigned to degenerate stretching, v3′t2 and degenerate deformation v4′t2 modes. The rather complex nuclear dynamics along the degenerate deformation mode, v4′t2, have been thoroughly investigated by Time-Dependent Density Functional Theory (TD-DFT) method. The relevant Jahn–Teller distortion operative within the lowest-lying electronic excited-state is shown here for the first time in order to yield a weak absorption feature at 6.156 eV. Further calculations on the potential energy curves for the singlet excited-states along the C–Cl stretching coordinate show the relevance of efficient C–Cl bond excision.

Biochemistry & Molecular Biology↗

DOE OSTI2024

Electronic Structure, Spectroscopy and Correlation Effects in Novel Materials

This project was targeted on electronic structure, spectroscopic studies, and correlation effects in a variety of novel materials of great current interest. Spectroscopies resolved highly in momentum, energy or spatial dimensions are playing a key role in unraveling the nature of the ground state and excitation properties in wide classes of novel materials. The seminal insights thus obtained are of critical importance not only for answering some of the fundamental questions facing condensed matter physics and materials science today, but also for understanding and thus helping to design and develop new materials with desirable properties, which will continue to be the key to the survival of mankind and its energy needs as a technological society long into the future. However, spectroscopies do not provide a direct map of electronic states, but act as a very complex ‘filter’ or ‘mapping’ of the underlying spectrum. This connection between the electronic states and measured spectra—called the ‘matrix element effect’—is in general an extremely complex function of the phase space of the experiment (e.g. energy/polarization of photons in photoemission), presenting both a challenge and an opportunity. So motivated, this project pursued techniques for realistic treatment of electronic spectra of a wide variety of materials, which served as a prelude to formulating and implementing methodologies for making direct connection with various spectroscopies such as ARPES, STS/STM, and inelastic light scattering. Specific systems are topological materials, including 2D ultrathin films beyond graphene, novel superconductors, and nanocrystals, among others. Our goal was to exploit the strengths of various spectroscopies to piece together the most complete picture of electronic states in systems of current interest, enabling direct and sharpened confrontations with theoretical models, and also to help advance the reach of various spectroscopies.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Toward Standardized Microscale Tensile Testing for Two‐Photon Polymerization‐Fabricated Materials in Liquid

Two-photon polymerization (TPP) enables the fabrication of intricate 3D microstructures with submicron precision, offering significant potential in biomedical applications like tissue engineering. In such applications, to print materials and structures with defined mechanics, it is crucial to understand how TPP printing parameters impact the material properties in a physiologically relevant liquid environment. Herein, an experimental approach utilizing microscale tensile testing (μTT) for the systematic measurement of TPP-fabricated microfibers submerged in liquid as a function of printing parameters is introduced. Using a diurethane dimethacrylate-based resin, the influence of printing parameters on microfiber geometry is first explored, demonstrating cross-sectional areas ranging from 1 to 36 μm 2 . Tensile testing reveals Young's moduli between 0.5 and 1.5 GPa and yield strengths from 10 to 60 MPa. The experimental data show an excellent fit with the Ogden hyperelastic polymer model, which enables a detailed analysis of how variations in writing speed, laser power, and printing path influence the mechanical properties of TPP microfibers. The μTT method is also showcased for evaluating multiple commercial resins and for performing cyclic loading experiments. Collectively, this study builds a foundation toward a standardized microscale tensile testing framework to characterize the mechanical properties of TPP printed structures.

mechanical characterization↗

NASA NTRS2003

The Chemistry and Excitation of Water in Molecular Clouds

We model the chemistry and thermal balance of opaque molecular clouds exposed to an external flux of ultraviolet photons. We include the processes of gas phase and grain surface chemical reactions; in particular we examine closely the freezing of atoms and molecules onto grain surfaces and the desorption of molecules from grain surfaces as a function of depth into a molecular cloud. We find that on the surface of a molecular cloud the gas phase water abundances are low because of photodissociation, and the grain phase water (ice) abundance is low because of photodesorption of water from the grain surfaces. Deeper into the cloud, at A(sub v) less than or approximately 2-8 depending on the strength of the external ultraviolet flux, the gas phase water abundance increases with depth as the photodissociation rates decline due to dust attenuation of the ultraviolet field. However, beyond A(sub v) less than or approximately 2-8 the gas phase water abundance declines because the water freezes as water ice on the grains, and photodesorption is no longer effective in clearing the ice. A peak water abundance of about 10(exp -6) to 10(exp -7) occurs at about A(sub v) approximately 2-8, relatively independent of the gas density and the ultraviolet field. We show that such a model matches very closely the observations of the Submillimeter Wave Astronomical Satellite (SWAS), a NASA Small Explorer Mission. The model elucidates several mechanisms that have been recently invoked to understand gas phase chemistry in clouds, including-the freeze-out of molecules onto grain surface, the desorption of these molecules from the surfaces, and the abundance gradients of molecules as functions of depth into molecular clouds.

Hollenbach, David↗