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At least 307 records · Page 17

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NASA NTRS2002

Measurement of Metastable Lifetimes of Highly-Charged Ions

The present work is part of a series of measurements of metastable lifetimes of highly-charged ions (HCIs) which contribute to optical absorption, emission and energy balance in the Interstellar Medium (ISM), stellar atmospheres, etc. Measurements were carried out using the 14-GHz electron cyclotron resonance ion source (ECRIS) at the JPL HCI facility. The ECR provides useful currents of charge states such as C(sup(1-6)+), Mg(sup(1-6)+) and Fe(sup(1-17)+). In this work the HCI beam is focused into a Kingdon electrostatic ion trap for measuring lifetimes via optical decays.

Smith, Steven J.↗

NASA NTRSDate not supplied

ACES Instrument

During the Atmospheric Carbon and Transport–America (ACT–America) suborbital mission (ACT-America) Mission Spring 2018 campaign, ASCENDS CarbonHawk Experiment Simulator (ACES), an intensity modulated continuous wave (IMCW) lidar system funded by NASA’s Science Mission Directorate, measured differential optical depths leading to partial-column CO2 lidar retrievals while flying aboard the C-130 aircraft across North America striving to advance technology critical to measuring column carbon dioxide mixing ratios (XCO2) remotely. ACES was developed by NASA Langley Research Center in the aims to have an active remote sensing system able to accurately measure XCO2 from space independent of the presence of sunlight, land surface type, and even through thin clouds. Differential absorption optical depth measurements made during the fourth campaign of ACT-America in Spring of 2018 were processed, analyzed and compared to on board in situ derived differential optical depth CO2 measurements.

XCO2↗

DOE OSTI2023

Enhanced Optical Contrast and Switching in Near‐Infrared Electrochromic Devices by Optimizing Conjugated Polymer Oligo(Ethylene Glycol) Sidechain Content and Gel Electrolyte Composition

Abstract A detailed investigation addressing the effects of functionalizing conjugated polymers with oligo(ethylene glycol) (EG n ) sidechains on the performance and polymer‐electrolyte compatibility of electrochromic devices (ECDs) is reported. The electrochemistry for a series of donor‐acceptor copolymers having near‐infrared (NIR)‐optical absorption, where the donor fragment is 3,4‐ethylenedioxythiophene (EDOT) or an EG n functionalized bithiophene (g2T) and the acceptor fragment is diketopyrrolopyrrole (DPP) functionalized with branched alkyl or EG n sidechains, is extensively probed. ECDs are next fabricated and it is found that EG n sidechain incorporation must be finely balanced to promote polymer‐electrolyte compatibility and provide efficient ion exchange. Proper electrolyte‐cation pairing and polymer structural tuning affords a 2x increase in optical contrast (from 12% to 24%) and >60x reduction in switching time (from 20 to 0.3 s). Atomic force microscopy (AFM)/grazing incidence wide‐angle X‐ray scattering (GIWAXS) characterization of the polymer film morphology/microstructure reveals that an over‐abundance of EG n sidechains generates large polymer crystallites, which can suppress ion exchange. Lastly, time‐of‐flight secondary ion mass spectrometry (ToF‐SIMS) indicates sidechain/electrolyte identity does not influence the electrolyte penetration depth into the films, and EG n sidechain inclusion increases electrolyte cation uptake. The material structural design insight and guidelines regarding the polymer‐electrolyte ion insertion/expulsion dynamics reported here should be of significant utility for developing next‐generation mixed ionic‐electronic conducting materials.

Chemistry↗

NASA NTRS2016

Optical Evaluation of DMDs with UV-Grade FS, Sapphire, MgF2 Windows and Reflectance of Bare Devices

Digital Micro-mirror Devices (DMDs) have been identified as an alternative to microshutter arrays for space-based multi-object spectrometers (MOS). Specifically, the MOS at the heart of a proposed Galactic Evolution Spectroscopic Explorer (GESE) that uses the DMD as a reprogrammable slit mask. Unfortunately, the protective borosilicate windows limit the use of DMDs in the UV and IR regimes, where the glass has insufficient throughput. In this work, we present our efforts to replace standard DMD windows with custom windows made from UV-grade fused silica, Low Absorption Optical Sapphire (LAOS) and magnesium fluoride. We present reflectance measurements of the antireflection coated windows and a reflectance study of the DMDs active area (window removed). Furthermore, we investigated the long-term stability of the DMD reflectance and recoating device with fresh Al coatings.

Quijada, Manuel A.↗

NASA NTRS1975

Measurements of SO2 absorption coefficients using a tunable dye laser

High-resolution measurements of SO2 absorption coefficients in the UV are presented in the wavelength interval between 2962 and 3011 A using a frequency-doubled dye laser as the radiation source. These measurements have application to pollution monitoring of SO2 using the differential absorption scattering (DAS) technique. The spectral resolution of the measurements was 0.2 A (determined by the linewidth of the dye laser) and the generated spectra exhibited considerable rotational structure on the (000) double prime to (060) prime, (070) prime, and (080) prime electronic-vibrational transitions. The latter transitions correspond to center wavelengths of 3001.8, 2981.0, and 2962 A, respectively. The laser measurements were obtained with a signal-processing technique which eliminated calibration procedures associated with conventional optical-absorption measurements. Using this technique, the statistical uncertainty associated with measured absorption coefficients has been reduced to less than plus or minus 2% with a wavelength uncertainty of the laser source of plus or minus 0.1 A.

Thompson, R. T., Jr.↗

NASA NTRS2013

A Bottom-Up Engineered Broadband Optical Nanoabsorber for Radiometry and Energy Harnessing Applications

Optical absorbers based on vertically aligned multi-walled carbon nanotubes (MWCNTs), synthesized using electric-field assisted growth, are described here that show an ultra-low reflectance, 100X lower compared to Au-black from wavelength lamba approximately 350 nm - 2.5 micron. A bi-metallic Co/Ti layer was shown to catalyze a high site density of MWCNTs on metallic substrates and the optical properties of the absorbers were engineered by controlling the bottom-up synthesis conditions using dc plasma-enhanced chemical vapor deposition (PECVD). Reflectance measurements on the MWCNT absorbers after heating them in air to 400deg showed negligible changes in reflectance which was still low, approximately 0.022 % at lamba approximately 2 micron. In contrast, the percolated structure of the reference Au-black samples collapsed completely after heating, causing the optical response to degrade at temperatures as low as 200deg. The high optical absorption efficiency of the MWCNT absorbers, synthesized on metallic substrates, over a broad spectral range, coupled with their thermal ruggedness, suggests they have promise in solar energy harnessing applications, as well as thermal detectors for radiometry.

optical absorbers↗

DOE OSTI2024

Broken Symmetry Optical Transitions in (6,5) Single-Walled Carbon Nanotubes Containing sp 3 Defects Revealed by First-Principles Theory

We present a first-principles many-body perturbation theory study of nitrophenyl-doped (6,5) single-walled nanotubes (SWCNTs) to understand how sp 3 doping impacts the excitonic properties. sp 3 -doped SWCNTs are promising as a class of optoelectronic materials with bright tunable photoluminescence, long spin coherence, and single-photon emission (SPE), motivating the study of spin excitations. We predict that the dopant results in a single unpaired spin localized around the defect site, which induces multiple low-energy excitonic peaks. By comparing optical absorption and photoluminescence from experiment and theory, we identify the transitions responsible for the red-shifted, defect-induced E 11 * peak, which has demonstrated SPE for some dopants; the presence of this state is due to both the symmetry-breaking associated with the defect and the presence of the defect-induced in-gap state. Furthermore, we find an asymmetry between the contribution of the two spin channels, suggesting that this system has potential for spin-selective optical transitions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS2002

Continuous pH monitoring in a perfused bioreactor system using an optical pH sensor

Monitoring and regulating the pH of the solution in a bioprocess is one of the key steps in the success of bioreactor operation. An in-line optical pH sensor, based on the optical absorption properties of phenol red present in the medium, was developed and tested in this work for use in NASA space bioreactors based on a rotating wall-perfused vessel system supporting a baby hamster kidney (BHK-21) cell culture. The sensor was tested over three 30-day and one 124-day cell runs. The pH sensor initially was calibrated and then used during the entire cell culture interval. The pH reported by the sensor was compared to that measured by a fiber optically coupled Shimadzu spectrophotometer and a blood gas analyzer. The maximum standard error of prediction for all the four cell runs for development pH sensor against BGA was +/-0.06 pH unit and for the fiber optically coupled Shimadzu spectrophotometer against the blood gas analyzer was +/-0.05 pH unit. The pH sensor system performed well without need of recalibration for 124 days. Copyright 2002 Wiley Periodicals, Inc.

Bioreactors↗

DOE OSTI2026

Direct Observation of Ultrafast Defect-Bound and Free Exciton Dynamics in Defect-Engineered WS 2 Monolayers

Defects in two-dimensional transition metal dichalcogenides (TMDCs) broadly affect their optical and electronic properties. Directly capturing the ultrafast processes of exciton trapping and defect-bound exciton formation is crucial for understanding and advancing defect-mediated optoelectronics and quantum technologies. However, the weak transient optical absorption of defect-bound excitons has limited their experimental observation to date. Here, we report the direct observation of the ultrafast dynamics of defect-bound excitons in monolayer WS 2 crystals with a high density of monosulfur vacancies (V S ) and W-site defect complexes (S W V S ) resulting from synthesis by alkali metal halide-assisted chemical vapor deposition. The dynamics of excitons bound to these defects, along with their coherent interactions with free excitons, are elucidated using ultrafast optical spectroscopy. Using above band-edge photoexcitation, we find that both free and defect-bound excitons simultaneously form within 300 fs from hot carrier relaxation. The defect-bound excitons exhibit shorter lifetimes than free excitons, leading to a population difference of the corresponding excitonic states and free exciton trapping within a 1–100 ps window. Band-edge photoexcitation of free and defect-bound exciton states reveals ultrafast interconversion within ∼150 fs (comparable to our temporal resolution), indicating possible coherent coupling between these states. We further demonstrate efficient up-conversion of defect-bound excitons to free excitons with photon energies up to ∼300 meV below the free exciton resonance. In conclusion, these findings provide insights into the ultrafast dynamics of defect-bound excitons in TMDCs and their coupling with free excitons, which are relevant to defect-engineered optoelectronic, quantum photonic, and valleytronic applications.

36 MATERIALS SCIENCE↗

NASA NTRS1991

Aerodyne Research mobile infrared methane monitor

An improved real-time methane monitor based on infrared absorption of the 3.39 micron line of a HeNe laser is described. Real time in situ measurement of methane has important applications in stratospheric and tropospheric chemistry, especially when high accuracy measurements can be made rapidly, providing fine spatial-scale information. The methane instrument provides 5 ppb resolution in a 1 sec averaging time. A key feature in this instrument is the use of magnetic (Zeeman) broadening to achieve continuous tunability with constant output power over a range of 0.017/cm. The instruments optical absorption path length is 47 m through sampled air held at 50 torr in a multipass cell of the Herriott (off-axis resonator) type. A microprocessor controls laser frequency and amplitude and collects data with minimal operator attention. The instrument recently has been used to measure methane emissions from a variety of natural and artificial terrestrial sources.

Mcmanus, J. B.↗

DOE OSTI2022

Beta Radiation Hardness of GYGAG(Ce) Transparent Ceramic Scintillators

GYGAG(Ce) transparent ceramic garnet scintillators were irradiated with electrons from 0.5 to 2 MeV with fluences from 10 16 e – /cm 2 to 10 19 e – /cm 2 , corresponding to doses from 0.3 to 310 Gigarad. Absorption spectra were measured before and after irradiations. Light yields from alpha, beta, and gamma excitations were measured before and after irradiation and compared to preirradiation values to gain a deeper understanding of how electron irradiations can affect light yield, as well as defects generated in both the surface and bulk. Within experimental error, no degradation in light yield was observed for the electron-irradiated samples, as measured via beta or gamma excitation, with minimal degradation observed via alpha excitation. A small increase in optical absorption near the wavelength of emission was observed following the largest dose irradiation. These results suggest that GYGAG(Ce) is radiation hard to electron irradiation up to 10 19 e – /cm 2 and doses up to 310 Gigarad. Furthermore, this robustness to irradiation indicates that transparent ceramic garnets may prove useful for applications such as scintillation-based nuclear batteries by allowing for higher energy beta emitters, increased power densities, and enabling long service lifetimes.

36 MATERIALS SCIENCE↗

NASA NTRS1991

Optical transitions in diamond at ultrahigh pressures

Optical studies on diamond at ultrahigh pressures are described which show that the unique properties of diamonds are affected by such stresses. Spectroscopic measurements show that the optical absorption edge shifts from UV to red with increasing pressures, and Raman scattering measurements how evidence for new structural transitions associated with large macroscopic deformation, beginning at a pressure of about 150 GPa. The changes are reversible and are associated with intense luminescence peaks at 2.0-2.2 eV under 458-514 nm radiation. These results may be related to the onset of bandgap closure in the approach to a new high-pressure phase. These spectral features must also be taken into account when diamond is used as optical windows for ultrahigh-pressure investigations.

Mao, H. K.↗

DOE OSTI2022

Unconventional optical properties of 2D Janus SMoSe induced by structural asymmetry

The Janus SMoSe monolayer that is best-known for its structural asymmetry is found to exhibit unconventional optical properties compared with its counterpart MoSe 2 . Optical transmittance measurements on monolayers that are directly synthesized on sapphire substrates reveal that the transmittance, as well as the real and imaginary parts of the optical dielectric constants of Janus SMoSe obtained from the Kramers–Kronig constrained analysis, show strong dependence on the polarization direction of the incident light. Meanwhile, the transmittance of the unpolarized light of Janus SMoSe becomes insensitive to light at incident angles up to 30°. The intrinsic dipoles induced by the structural asymmetry of Janus SMoSe are believed to produce these distinct optical properties. Finally, by estimating the optical absorption of the intrinsic dipoles and tracing their dependence on the light incident angles, we speculate that the dipoles are not perpendicularly aligned to the in-plane direction of the monolayer, but rather tilted by a small angle between 0° and 10°.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Revealing Parallel Inter‐ and Intra‐Ligand Charge Transfer Dynamics in [Ru(L) 2 (dppz)] 2+ Molecular Lightswitch with N K‐Edge X‐Ray Absorption Spectroscopy

In photoactive metal complexes the localization of photoexcited charges dictates the site of chemical reactivity, but few studies measure the charge redistribution in these systems with spatial precision. Herein, we track the inter- and intra-ligand charge transfer processes that underpin light-driven charge separation in the well-studied “molecular lightswitch” [Ru(bpy) 2 dppz] 2+ (aqueous [Ruthenium II (2,2′-bipyridine)2(dipyrido[3,2-a:2′,3′-c]phenazine)] 2+ [Cl − ] 2 ) by probing the electronic structure of ligand nitrogen atoms in real-time using ultrafast X-ray absorption spectroscopy and first principles calculations. We confirm the localization of excited electron density on the phenazine N atoms of dppz and we newly identify two parallel electron transfer pathways to populate this state. Sub-70 fs electron transfer to the phenazine portion of dppz is observed and attributed to intra-ligand electron transfer following Ru-to-dppz metal-to-ligand charge transfer (MLCT) excitation. This fast charge transfer was not reported in prior ultrafast studies. The slower (ca. 2 ps) charge transfer reported extensively in time-resolved optical absorption and emission studies is reassigned here to inter-ligand electron “hopping” between nearly isoenergetic ligand moieties following Ru-to-bpy MLCT excitation. In conclusion, the results demonstrate much faster charge separation than previously identified in this well-studied system, highlighting how extended azaacene ligand motifs promote the competitive charge transfer processes needed to drive light-driven electron transfer chemistry.

Donor-acceptor systems↗

DOE OSTI2025

Computational and Experimental Investigation of Chiral and Achiral Two‐Dimensional Organic Lead Bromide Perovskites: Octahedral Distortions and Electronic and Optical Properties

A computational investigation is presented, in conjunction with synthesis and experimental characterization, into the structural, electronic, and optical properties of layered two-dimensional organic lead bromide perovskites. Materials based on the chiral (R/S)-4-fluoro-α-methylbenzylammonium (R/S-FMBA), which have been shown to lead to bright room-temperature circularly polarized luminescence, are contrasted with the similar achiral 4-fluorobenzylammonium (FBA). Using density functional theory (DFT) with van der Waals (vdW) corrections, relaxed structures (compared with X-ray diffraction, XRD) and optical absorption spectra (compared with experiments) are studied, as well as band structure and orbital character of transitions. A Python code is developed and provided to calculate octahedral distortions and compare DFT and XRD results, finding that vdW corrections are important for accuracy and that DFT overestimates octahedral tilt angles. (FMBA) 2 PbBr 4 shows among the largest tilt angle differences (often termed Δ β ) reported, 14°–15°, indicating strong inversion symmetry-breaking, which enables its chiral emission. A large resulting Dresselhaus spin-splitting effect is found. The lowest-energy optical transitions involve the perovskite only and are polarized within the layer. This work furthers understanding of structure-property relations with applications to optoelectronics and spintronics.

UV/vis spectroscopy↗

DOE OSTI2022

Spinor $GW$ Bethe-Salpeter calculations in BerkeleyGW: Implementation, symmetries, benchmarking, and performance

Computing the GW quasiparticle band structure and Bethe-Salpeter equation (BSE) absorption spectra for materials with spin-orbit coupling have commonly been done by treating GW corrections and spin-orbit coupling (SOC) as separate perturbations to density-functional theory. However, accurate treatment of materials with strong spin-orbit coupling (such as many topological materials of recent interest, and thermoelectrics) often requires a nonperturbative approach using spinor wave functions in the Kohn-Sham equation and GW/BSE. Such calculations have only recently become available, in particular for the BSE. Here, we have implemented this approach in the plane-wave pseudopotential GW/BSE code BerkeleyGW, which is highly parallelized and widely used in the electronic-structure community. We present reference results for quasiparticle band structures and optical absorption spectra of solids with different strengths of spin-orbit coupling, including Si, Ge, GaAs, GaSb, CdSe, Au, and Bi 2 Se 3 . The calculated quasiparticle band gaps of these systems are found to agree with experiment to within a few tens of meV. SOC splittings are found to be generally in better agreement with experiment, including quasiparticle corrections to band energies. The absorption spectrum of GaAs is not significantly impacted by the inclusion of spin-orbit coupling due to its relatively small value (0.2 eV) in the Λ direction, while the absorption spectrum of GaSb calculated with the spinor GW/BSE captures the large spin-orbit splitting of peaks in the spectrum. For the prototypical topological insulator Bi 2 Se 3 , we find a drastic change in the low-energy band structure compared to that of DFT, with the spinorial treatment of the GW approximation correctly capturing the parabolic nature of the valence and conduction bands after including off-diagonal self-energy matrix elements. We present the detailed methodology, approach to spatial symmetries for spinors, comparison against other codes, and performance compared to spinless GW/BSE calculations and perturbative approaches to SOC. This work aims to spur further development of spinor GW/BSE methodology in excited-state research software and enables a more accurate and detailed exploration of electronic and optical properties of materials containing elements with large atomic numbers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

NASA NTRS1991

Grooved surfaces on InP

Formation of a textured or grooved front surface on a solar cell can increase the efficiency in several ways, including enhanced absorption and light trapping. In III-IV materials the (111) plane is chemically different form the (1'1'1') plane, and both etching and epitaxial deposition behave differently on these surfaces. The current state of profile etching in InP is summarized. Data are presented on novel geometries attainable as a function of etchant temperature and composition, substrate orientation and carrier concentration, and the oxide thickness between the substrate and the photoresist. Depending on dopant concentration, the same etchant can produce either anisotropic or isotropic grooves. V-grooved solar cells were manufactured on InP, and the improved optical absorption was demonstrated. Preferred parameters for various applications are listed and discussed.

Bailey, Sheila G.↗

DOE OSTI2024

Development of AlGaN‐Based Deep‐Ultraviolet Avalanche Photodetectors—Toward Their Intrinsic Characteristics

Al 0.6 Ga 0.4 N deep‐UV p–i–n avalanche photodiodes (APDs) are demonstrated grown by metalorganic chemical vapor deposition (MOCVD) on a (0001) c‐plane aluminum nitride (AlN) bulk substrate and fabricated both with and without an ion implantation process for mesa‐edge electric‐field termination. Three design considerations are taken into account: the optical absorption of the AlN bulk substrate, the photosensitivity of the APD, and the breakdown electric field. The MOCVD growth conditions of the AlGaN APD layers are optimized. Then, a detailed description of the seven device fabrication steps of the APDs is provided, which includes nitrogen ion implantation. The APDs fabricated by the ion implant process exhibit a dark‐current density under low reverse bias ≈1 × 10 −9 A cm −2 . This is one order of magnitude lower than the APD fabricated without ion implantation from the same wafer. The breakdown voltage of the APD is ≈−140 V. The calculated optical gain of the ion‐implanted APD beyond avalanche breakdown is ≈5.2 × 10 5 (current limited) and the device has an average zero‐bias photoresponse of ≈68 mA W −1 at a wavelength of 250 nm.

Jeong, Hoon [Department of Electronic Engineering ↗