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At least 577 records · Page 32
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Spectroscopy in Nanoscopic Cavities: Models and Recent Experiments

The ability of nanophotonic cavities to confine and store light to nanoscale dimensions has important implications for enhancing molecular, excitonic, phononic, and plasmonic optical responses. Spectroscopic signatures of processes that are ordinarily exceedingly weak such as pure absorption and Raman scattering have been brought to the single-particle limit of detection, while new emergent polaritonic states of optical matter have been realized through coupling material and photonic cavity degrees of freedom across a wide range of experimentally accessible interaction strengths. In this review, we discuss both optical and electron beam spectroscopies of cavity-coupled material systems in weak, strong, and ultrastrong coupling regimes, providing a theoretical basis for understanding the physics inherent to each while highlighting recent experimental advances and exciting future directions.

Chemistry↗
DOE OSTI2021

Electro-Optical Measurement Techniques

Utilize the unique characteristics of photons across different regions of the electromagnetic spectrum to probe the optical and electronic properties of chemical systems, materials and devices for energy conversion technologies.

absorption↗
DOE OSTI2022

Redshift evolution of the H I detection rate in radio-loud active galactic nuclei

We present a search for associated H I 21 cm absorption in a sample of 29 radio-loud active galactic nuclei (AGNs) at 0.7 < z < 1, carried out with the upgraded Giant Metrewave Radio Telescope. We detect H I 21 cm absorption against none of our target AGNs, obtaining 3σ upper limits to the optical depth of ≲1% per 50 km s –1 channel. The radio luminosity of our sources is lower than that of most AGNs searched for H I 21 cm absorption at similar redshifts in the literature, and, for all targets except two, the UV luminosity is below the threshold 10 23 W Hz –1 , above which the H I in the AGN environment has been suggested to be completely ionised. We stacked the H I 21 cm spectra to obtain a more stringent limit of ≈0.17% per 50 km s –1 channel on the average H I 21 cm optical depth of the sample. Furthermore, the sample is dominated by extended radio sources, 24 of which are extended on scales of tens of kiloparsecs. Including similar extended sources at 0.7 < z < 1.0 from the literature, and comparing with a low-z sample of extended radio sources, we find statistically significant (≈3σ) evidence that the strength of H I 21 cm absorption towards extended radio sources is weaker at 0.7 < z < 1.0 than at z < 0.25, with a lower detection rate of H I 21 cm absorption at 0.7 < z < 1.0. Redshift evolution in the physical conditions of H I is the likely cause of the weaker associated H I 21 cm absorption at high redshifts, due to either a low H I column density or a high spin temperature in high-z AGN environments.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

FLASH pilot survey: detections of associated 21 cm H i absorption in GAMA galaxies at 0.42 < z < 1.00

ABSTRACT We present the results of a search for associated 21 cm H i absorption at redshift 0.42 < z < 1.00 in radio-loud galaxies from three Galaxy And Mass Assembly (GAMA) survey fields. These observations were carried out as part of a pilot survey for the Australian SKA Pathfinder (ASKAP) First Large Absorption Survey in H i (FLASH). From a sample of 326 radio sources with 855.5 MHz peak flux density above 10 mJy, we detected two associated H i absorption systems, in SDSS J090331+010847 at z = 0.522 and SDSS J113622+004852 at z = 0.563. Both galaxies are massive (stellar mass $\gt 10^{11}\, \mathrm{M}_\odot$) and have optical spectra characteristic of luminous red galaxies, though spectral energy distribution fitting implies that SDSS J113622+004852 contains a dust-obscured starburst with star formation rate ∼69 M⊙ yr−1. The H i absorption lines have a high optical depth, with τpk of 1.77 ± 0.16 for SDSS J090331+010847 (the highest value for any z > 0.1 associated system found to date) and 0.14 ± 0.01 for SDSS J113622+004852. In the redshift range probed by our ASKAP observations, the detection rate for associated H i absorption lines (with τpk > 0.1 and at least 3σ significance) is $2.9_{-2.6}^{+9.7}$ per cent. Although the current sample is small, this rate is consistent with a trend seen in other studies for a lower detection rate of associated 21 cm H i absorption systems at higher redshift. We also searched for OH absorption lines at 0.67 < z < 1.34, but no detection was made in the 145 radio sources searched.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2021

Visible-light Phase Curves from the Second Year of the TESS Primary Mission

We carried out a systematic study of full-orbit phase curves for known transiting systems in the northern ecliptic sky that were observed during Year 2 of the TESS primary mission. We applied the same methodology for target selection, data processing, and light-curve fitting as we did in our Year 1 study. Out of the 15 transiting systems selected for analysis, seven—HAT-P-7, KELT-1, KELT-9, KELT-16, KELT-20, Kepler-13A, and WASP-12—show statistically significant secondary eclipses and day–night atmospheric brightness modulations. Small eastward dayside hot-spot offsets were measured for KELT-9b and WASP-12b. KELT-1, Kepler-13A, and WASP-12 show additional phase-curve variability attributed to the tidal distortion of the host star; the amplitudes of these signals are consistent with theoretical predictions. We combined occultation measurements from TESS and Spitzer to compute dayside brightness temperatures, TESS-band geometric albedos, Bond albedos, and phase integrals for several systems. The new albedo values solidify the previously reported trend between dayside temperature and geometric albedo for planets with 1500 K < T {sub day} < 3000 K. For Kepler-13Ab, we carried out an atmospheric retrieval of the full secondary eclipse spectrum, which revealed a noninverted temperature–pressure profile, significant H{sub 2}O and K absorption in the near-infrared, evidence for strong optical atmospheric opacity due to sodium, and a confirmation of the high geometric albedo inferred from our simpler analysis. We explore the implications of the phase integrals (ratios of Bond to geometric albedos) for understanding exoplanet clouds. We also report updated transit ephemerides for all of the systems studied in this work.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Elucidating the Role of Hydrogen Bonding in the Optical Spectroscopy of the Solvated Green Fluorescent Protein Chromophore: Using Machine Learning to Establish the Importance of High-Level Electronic Structure

Hydrogen bonding interactions with chromophores in chemical and biological environments play a key role in determining their electronic absorption and relaxation processes, which are manifested in their linear and multidimensional optical spectra. For chromophores in the condensed phase, the large number of atoms needed to simulate the environment has traditionally prohibited the use of high-level excited-state electronic structure methods. By leveraging transfer learning, we show how to construct machine-learned models to accurately predict the high-level excitation energies of a chromophore in solution from only 400 high-level calculations. Here, we show that when the electronic excitations of the green fluorescent protein chromophore in water are treated using EOM-CCSD embedded in a DFT description of the solvent the optical spectrum is correctly captured and that this improvement arises from correctly treating the coupling of the electronic transition to electric fields, which leads to a larger response upon hydrogen bonding between the chromophore and water.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

The frequency of extreme X-ray variability for radio-quiet quasars

ABSTRACT We analyse 1598 serendipitous Chandra X-ray observations of 462 radio-quiet quasars to constrain the frequency of extreme amplitude X-ray variability that is intrinsic to the quasar corona and innermost accretion flow. The quasars in this investigation are all spectroscopically confirmed, optically bright (mi ≤ 20.2), and contain no identifiable broad absorption lines in their optical/ultraviolet spectra. This sample includes quasars spanning z ≈ 0.1–4 and probes X-ray variability on time-scales of up to ≈12 rest-frame years. Variability amplitudes are computed between every epoch of observation for each quasar and are analysed as a function of time-scale and luminosity. The tail-heavy distributions of variability amplitudes at all time-scales indicate that extreme X-ray variations are driven by an additional physical mechanism and not just typical random fluctuations of the coronal emission. Similarly, extreme X-ray variations of low-luminosity quasars seem to be driven by an additional physical mechanism, whereas high-luminosity quasars seem more consistent with random fluctuations. The amplitude at which an X-ray variability event can be considered extreme is quantified for different time-scales and luminosities. Extreme X-ray variations occur more frequently at long time-scales (Δt ≳ 300 d) than at shorter time-scales and in low-luminosity quasars compared to high-luminosity quasars over a similar time-scale. A binomial analysis indicates that extreme intrinsic X-ray variations are rare, with a maximum occurrence rate of $\lt 2.4{{\ \rm per\ cent}}$ of observations. Finally, we present X-ray variability and basic optical emission-line properties of three archival quasars that have been newly discovered to exhibit extreme X-ray variability.

Timlin, III, John D.↗
DOE OSTI2024

Transient fading X-ray emission detected during the optical rise of a tidal disruption event

ABSTRACT We report on the SRG/eROSITA detection of ultra-soft ($kT=47^{+5}_{-5}$ eV) X-ray emission (LX =$2.5^{+0.6}_{-0.5} \times 10^{43}$ erg s−1) from the tidal disruption event (TDE) candidate AT 2022dsb ∼14 d before peak optical brightness. As the optical luminosity increases after the eROSITA detection, then the 0.2–2 keV observed flux decays, decreasing by a factor of ∼39 over the 19 d after the initial X-ray detection. Multi-epoch optical spectroscopic follow-up observations reveal transient broad Balmer emission lines and a broad He ii 4686 Å emission complex with respect to the pre-outburst spectrum. Despite the early drop in the observed X-ray flux, the He ii 4686 Å complex is still detected for ∼40 d after the optical peak, suggesting the persistence of an obscured hard ionizing source in the system. Three outflow signatures are also detected at early times: (i) blueshifted H α emission lines in a pre-peak optical spectrum, (ii) transient radio emission, and (iii) blueshifted Ly α absorption lines. The joint evolution of this early-time X-ray emission, the He ii 4686 Å complex, and these outflow signatures suggests that the X-ray emitting disc (formed promptly in this TDE) is still present after optical peak, but may have been enshrouded by optically thick debris, leading to the X-ray faintness in the months after the disruption. If the observed early-time properties in this TDE are not unique to this system, then other TDEs may also be X-ray bright at early times and become X-ray faint upon being veiled by debris launched shortly after the onset of circularization.

Malyali, A. (ORCID:0000000288514019)↗
DOE OSTI2020

Hollow fiber mid-ID spectrometer with UV laser ablation sampling for fine spatial reoslution of isotope ratios in solids

We describe a system that combines isotope ratio analysis via mid-infrared (Mid-IR) laser absorption spectroscopy with fine spatial resolution sampling using a UV pulsed laser. The UV laser ablates a pit in a solid on the order of 10 microns in diameter. The sample-derived particulates resulting from laser ablation pass through a micro-combustor, and the resulting gas is analyzed using Mid-IR laser absorption spectroscopy in a capillary absorption spectrometer (CAS). The CAS uses a hollow fiber optic waveguide with a reflective inner coating and a small internal volume on the order of 1ml. The hollow fiber both guides the laser light from source to detector and contains the gas sample at reduced pressure. Near unity overlap between the laser beam and sample enables sensitive analysis with ultra-small sample size. A prototype system has been demonstrated to enable stable carbon isotopic analysis (d13C) with 1 per mil precision using <1 picomole of carbon and is currently being used to study nutrient exchange in soil/root/microbial rhizosphere studies. The smaller sample size of this system is enabling fine spatial resolution analysis (on the order of 10 microns), which is roughly an order of magnitude smaller than was possible with an isotope ratio mass spectrometer (IRMS). In addition to rhizosphere studies, the system can provide a useful tool for fine scale isotope analysis with applications in biological, forensic, and environmental science.

capillary absorption spectroscopy, laser ablation,↗
DOE OSTI2023

Chiral Spectroscopy of Nanostructures

Chirality is ubiquitous in the universe and in living creatures over detectable length scales from the subatomic to the galactic, as exemplified in the two extremes by subatomic particles (neutrinos) and spiral galaxies. Between them are living creatures that display multiple levels of chirality emerging from hierarchically assembled asymmetric building blocks. Not too far from the bottom of this pyramid are the foundational building blocks with chiral atomic centers on sp 3 carbon atoms exemplified by L-amino acids and D-sugars that are self-assembled into higher-order structures with increasing dimensions forming highly complex, amazingly functional, and energy-efficient living systems. The organization and materials employed in their construction inspired scientists to replicate complex living systems via the self-assembly of chiral components. Multiple studies pointed to unexpected and unique electromagnetic properties of chiral structures with nanoscale and microscale dimensions, including giant circular dichroism and collective circularly polarized scattering that their constituent units did not possess. To address the wide variety of chiral geometries observed in continuous materials, singular particles, and their complex systems, multiple analytic techniques are needed. Simultaneously, their spectroscopic properties create a pathway to multiple applications. For example, mirror-asymmetric vibrations at chiral centers formed by sp 3 carbon atoms lead to optical activity for the infrared (IR) wavelength regions. At the same time, understanding the optical activity in, for example, the IR region enables biomedical applications because multiple modalities of biomedical imaging and vibrational optical activity (VOA) of biomolecules are known for IR range. In turn, VOA can be realized in both absorption and emission modalities due to large magnetic transition moments, as vibrational circular dichroism (VCD) or Raman optical activity (ROA) spectroscopy. In addition to the VOA, in the range of longer wavelengths, lattice vibrational mode or phononic behavior occurs in chiral crystals and nanoassemblies, which can be readily detected by terahertz circular dichroism (TCD) spectroscopy. Meanwhile, chiral self-assembly can induce circularly polarized light emission (CPLE) regardless of the existence of chirality in coassembled fluorophores. The CPLE from self-assembled chiral materials is particularly interesting because the CPLE can originate from both circularly polarized luminescence and circularly polarized scattering (CPS). Furthermore, because self-assembled nanostructures often exhibit stronger optical activity than their building blocks owing to dimension and resonance effects, the optical activity of single assembled nanostructures can be investigated by using microscopic technology combined with chiral optics. Here, we describe the state of the art for spectroscopic methods for the comprehensive analysis of chiral nanomaterials at various photon wavelengths, addressed with special attention given to new tools emerging both for materials with self-organized hierarchical chirality and single-particle spectroscopy.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Unabsorbed light beamlets for diagnosing coronal density profiles and absorption nonuniformity in direct-drive implosions on OMEGA

Laser light scattered from a target is the most-direct measurement for diagnosing laser absorption in a direct-drive implosion. The 3ωGOI (gated optical imager) beamlets diagnostic images unabsorbed light from all 60 OMEGA beams as distinct “beamlet” spots for each beam. The implosion can be diagnosed using the position and intensity of these beamlets. The position of each beamlet in the image is determined by refraction and can be used to fit the coronal plasma density profile of the implosion. The inferred plasma density profiles are comparable to profiles predicted by the 1-D hydrodynamics code LILAC but suggest the predictions underestimate the density farther out in the corona. The intensity of light in each spot depends on the cumulative effects of absorption and cross-beam energy transfer along the beamlet’s path through the corona. Furthermore, the measured variation in intensity and polarization between similar spots indicates that absorption during OMEGA implosions is less uniform than previously known.

47 OTHER INSTRUMENTATION↗
DOE OSTI2022

Optimizing molecular light absorption in the strong coupling regime for solar energy harvesting

The strong coupling of optical absorbers (e.g., molecules or semiconductors) to confined photonic modes fundamentally alters the physical properties of the coupled system via the formation of hybrid light-matter states. One potential application of strong light-matter coupling relies on exploiting it to localize light-induced charge excitation processes to small volumes of material. Applications that would benefit from this localization include thin-film photovoltaics, photodetection, photocatalysis, and others, where the overall performance depends on the ability of a material to amplify light absorption (i.e., the formation of electron-hole pairs) within specific locations in space. This contribution investigates how strong light-matter coupling affects light absorption rates in molecular absorbers coupled to photonic nanostructures. Here, our results show that the molecular light absorption efficiencies are highest in configurations where the strongly coupled molecules interact directly with the incoming photon flux. We also identify a nonlinear dependence in the molecular absorption as a function of concentration, unique to the strongly coupled systems. Based on these results, we propose design principles for engineering nanostructured systems that allow for high efficiencies of charge carrier localization into strongly coupled absorbers.

14 SOLAR ENERGY↗
DOE OSTI2024

Electronic, direct optical, and phonon-assisted optical properties of 4H Si from first principles

The cubic polytype of silicon (Si) is the most commercialized semiconductor material and finds applications in numerous electronic and optoelectronic devices, such as solar cells. However, recent reports on the synthesis of the hexagonal 4H Si polytype have attracted the attention of the scientific community to understand its functional properties. Here, we report the electronic, vibrational, and optical properties of the 4H Si polytype obtained with predictive first-principles calculations, with an emphasis of phonon-assisted absorption in the indirect regime. Compared to the cubic polytype, 4H Si shows a slightly narrower indirect gap by ∼0.05 eV. The calculated phonon-assisted optical spectra show that 4H Si exhibits a stronger absorption coefficient than cubic Si across the visible and IR spectral regions. We further evaluate the short-circuit current density of textured thin-films. We demonstrate that 4H Si can achieve the same short-circuit current density for a five times thinner film compared to the cubic polytype, which mainly resulted from absorption in the indirect gap regime. Our work demonstrates the advantages of 4H Si for thin-film silicon-based solar-cell applications.

Materials Science↗
DOE OSTI2024

Laser absorptivity measurement device

A laser absorptivity measurement device uses a linearly polarized incident beam, an optical configuration comprising an internal polarizing beamsplitter that transmits the linearly polarized incident beam and a quarter-wave plate that converts linearly polarized incident beam into a circularly polarized incident beam that is reflected off a processing substrate. The quarter-wave plate and polarizing beamsplitter can then direct the reflected light back into an integrating volume, where the power of the reflected light can be measured by a photodetector. The laser absorptivity measurement device is capable of making real-time absorption efficiency measurements of a variety of laser-based processes, including laser welding and brazing, additive manufacturing, and laser marking.

Tung, Daniel↗
DOE OSTI2025

Spectroscopic Properties of Americium(III) in Mineral Acid Media

We report the preparation and optical characterization of three solutions of Am(III) in common aqueous (aq.) mineral acids (HCl, HNO 3 and HBr), including absorption, emission, and Raman vibrational analyses. To our knowledge, this study provides the first detailed absorption spectra of Am(III) spanning the entire UV/Vis/NIR region in these mineral acids reported since the 1960s. Here, using this high-resolution absorption data, provided in an open access format for the broader field, we build on prior work by Carnall and others to provide detailed optical analysis including all transition assignments. This work also includes the first reported absorption spectrum of Am(III) in aq. HBr. Characteristic Am(III) luminescence could be detected from all three samples. These are the first reports of emission from Am(III) in these acid systems, which build on prior emission reports collected from aq. HClO 4 solutions. The acquired emission spectra display anion-dependent shifting of the visible-region transitions by up to 21 nm from their predicted positions, akin to the nephelauxetic effect. The shift magnitude trends linearly according to the acid p K a and more generally according to the transition metal spectrochemical series. These ligand field effects, coupled with luminescence lifetime experiments, indicate that weak Am-X interactions persist in solution.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Interferometric two-photon-absorption spectroscopy with three entangled photons

In this work, we propose an interferometric pump-probe technique that employs three entangled photons generated by cascaded spontaneous parametric downconversion. A Mach–Zehnder interferometer made of two three-port waveguide arrays is inserted in the optical path. Two independent phases introduced to manipulate the entangled photon state serve as control parameters and can selectively excite matter pathways. Compared to two-photon-absorption of an entangled photon-pair, the three-photon signals are significantly enhanced by frequency-dispersed photon-counting detection.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Intrinsic Formamidinium Tin Iodide Nanocrystals by Suppressing the Sn(IV) Impurities

The long search for non-toxic alternatives to lead halide perovskites (LHPs) has shown that some compelling properties of LHPs, such as low effective masses of carriers, can only be attained in their closest Sn(II) and Ge(II) analogs, despite their tendency to oxidation. Judicious choice of chemistry allowed formamidinium tin iodide (FASnI 3 ) to reach a power conversion efficiency of 14.81% in photovoltaic devices. This progress motivated us to develop a synthesis of colloidal FASnI 3 NCs with a concentration of Sn(IV) reduced to an insignificant level and probe their intrinsic structural and optical properties. Intrinsic FASnI 3 NCs exhibit unusually low absorption coefficients of 4 x 10 3 cm -1 at the first excitonic transition, a 190 meV increase of the bandgap as compared to the bulk material, and a lack of excitonic resonances. These features are attributed to a highly disordered lattice, distinct from the bulk FASnI 3 as supported by structural characterizations and first-principles calculations.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2026

Mitigating Hydrogen-Induced Degradation of Iridium Anodes in Proton Exchange Membrane Water Electrolyzers

One promising method for reducing precious metal usage in proton exchange membrane water electrolysis is lowering iridium (Ir) loading at the anode. However, low-loading Ir catalysts often suffer from poor stability under high current densities. In this study, hydrogen (H2) crossover from the cathode to the anode is identified as a key degradation pathway. Temperature-programmed reduction confirms the reduction of IrO2 at 80 °C in a hydrogen environment, highlighting the vulnerability of IrO2-based catalysts to H2 exposure. To mitigate this effect, palladium (Pd) is introduced as an anode additive, acting as an H2 oxidation catalyst and mitigating IrO2 reduction. This protective role is verified by inductively coupled plasma optical emission spectroscopy and in situ X-ray absorption spectroscopy, showing significantly suppressed Ir dissolution at 80 °C under H2 flow when an O-covered Pd surface is present at oxygen evolution reaction potentials. Results from the current study identify a new strategy in improving activity and durability of catalysts in electrolyzers.

58 GEOSCIENCES↗