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NASA NTRSDate not supplied

Evaluating Diurnal Ozone Emissions: A Comparative Analysis of DSCOVR EPIC, PANDORA, and TOLNet Data for Space-Based Monitoring Assessment: A Case Study by ASDC

Stratospheric ozone occurs naturally in the upper atmosphere, forming a protective layer that shields us from the sun's harmful ultraviolet rays. Tropospheric ozone is not emitted directly into the air but is created by chemical reactions between nitrogen oxides (NOx) and volatile organic compounds (VOC). This reaction happens when pollutants emitted by cars, power plants, industrial boilers, refineries, chemical plants, and other sources chemically react in sunlight [1]. Therefore, increased levels of tropospheric ozone indicate the presence of pollutants in the air. While daily anthropogenic activity causes an increase of ground-level ozone, variation of stratospheric ozone changes happens much slower, so that variation of the total ozone column reflects the variation of the tropospheric column due to natural, e.g., wildfires and anthropogenic air pollution. Both total and tropospheric ozone column products are used in this study. The reflectance spectra measured by the Earth Polychromatic Imaging Camera (EPIC) instrument aboard the Deep Space Climate Observatory (DSCOVR) spacecraft are compared with a set of radiative transfer-derived lookup tables for the EPIC filter transmission functions and a wide range of ozone values to retrieve ozone with a maximum resolution of 18 km at the sub-satellite point [2]. EPIC provides total column ozone in level 2 and level 4 products and tropospheric column ozone in level 4 products. Both EPIC Ozone products [2] are available at the Atmospheric Science Data Center (ASDC) at NASA Langley Research Center [3, 4]. Pandora spectrometer instrument measures columnar amounts of trace gases in the atmosphere. These gases (O3, NO2, CH2O) absorb light from the sun at specific wavelengths in the ultraviolet-visible spectrum [5]. Using the theoretical solar spectrum as a reference, Pandora determines trace gas amounts using differential optical absorption spectroscopy (DOAS). Pandora ozone retrievals are available from the Pandonia Global Network [6]. Pandora data from North American major metropolitan areas, New York, NY, Washington DC, Los Angeles, CA, and Mexico City. Tropospheric Ozone Lidar Network (TOLNet) was established in 2012 to provide high spatiotemporal observations of tropospheric ozone to (1) better understand physical processes driving the ozone budget in various meteorological and environmental conditions and (2) validate the tropospheric ozone measurements of space-borne missions [7]. TOLNet data are available at ASDC [8]. While EPIC provides global coverage of ozone retrievals several times daily, temporal resolution may miss some features in daily ozone variations. Ground-based sensors such as Pandora spectrometers and TOLNet lidars provide better temporal resolution while missing continuous spatial coverage. The forthcoming ozone retrieval from the TEMPO mission [9] will provide better spatial and temporal coverage of air quality (including ozone) over North America. This study investigates whether EPIC ozone products can detect diurnal air quality variations and compare ozone temporal development with retrieval by ground-based instruments.

diurnal ozone emissions, DSCOVR EPIC, PANDORA, spa↗

NASA NTRSDate not supplied

Progress of 2.05 uM Fiber Laser Development for A Martian Co2 Dial

We have proposed a new concept for differential absorption lidar (DIAL) operating in the 2050 nm CO 2 absorption band for atmospheric CO 2 and pressure observations on Mars. This concept has earned us funding from NASA's PICASSO Program to advance 2050 nm fiber laser technology for future space applications. The laser design is an all-fiber master oscillator and power amplifier (MOPA) system. The master oscillator with pulse shaping and several stages of fiber preamplifiers has been built. Preliminary tests show the output pulse energy can reach 1 mJ, meeting our baseline goal. However, the current power amplifier design has an issue with undesired parasitic lasing at a different frequency, which exhausts pump energy and limits the laser energy. We have modified the power amplifier design to suppress parasitic lasing, and higher laser power energy is expected. To achieve high measurement accuracy, the laser frequency must be stabilized. A fraction of the master oscillator is split to lock the laser frequency to the center of the selected absorption line. The laser can then be shifted to a frequency far from the absorption line center, where extinction due to CO 2 and other trace gases is minimal, serving as the offline reference. The online wavelength is optimized at 2050.44156 nm, ensuring a CO 2 absorption optical depth (AOD) of approximately 1.1 at 3 km, which maximizes the signal-to-noise ratio (SNR) for measurements in the lower Martian atmosphere. At the conference, we will provide more details about this project and report on the progress of instrument development.

DIAL↗

DOE OSTI2016

Evaluating the oxidative, photothermal and electrical stability of colloidal nanocrystal solids

IV-VI quantum dot (QD) solids are a novel class of granular electronic materials with great technological potential (e.g., in photodetectors, field-effect transistors (FETs), and solar cells), but their oxidative and thermal instability present a barrier to practical applications [1]. Poor stability is a fundamental issue facing many nanoscale materials due to high surface area and surface energy. Basic studies are needed to elucidate the most important mechanisms of degradation and develop robust countermeasures if QD materials are to become technologically important. This project determined the degradation mechanisms of IV-VI QD solids (primarily PbSe and PbS) and introduced new chemical strategies to drastically improve their performance, stability, and operating lifetimes [2-5]. Our approach was based on (1) detailed testing of QD thin film materials (principally FETs and solar cells) as a function of oxidative and thermal stress, and (2) the use of organic and inorganic approaches to link the QDs into strongly electronically coupled, high-mobility films, prevent their oxidation, and eliminate internal degrees of freedom that lead to film instability and degradation in response to electrical and thermal stress. Stability against oxidation and thermal degradation was the major focus of this project. We have evaluated the stability of QD thin films and interfaces at temperatures less than 100°C (the regime most relevant to solar and transistor applications). Low-temperature oxidation and sintering of QD films have been investigated using optical absorption spectroscopy, Fourier transform infrared spectroscopy (FTIR), current-voltage scanning of transistors and solar cells, X-ray photoelectron spectroscopy, and scanning Kelvin probe microscopy (SKPM). SKPM was used to map the potential profiles of operating QD FETs and solar cells as a function of bias and illumination, which provides detailed information on how the work functions, potential drops and electric field within these devices determine device operation, and set the stage for future studies targeted at understanding and preventing device failure. We pursued two strategies to fabricate QD films with stable electrical characteristics: (1) the use of robust molecular surface ligands [2], and (2) “matrix engineering,” i.e., infilling the QD solid with metal oxide or metal sulfide matrices by low-temperature atomic layer deposition (ALD) to passivate surface states, prevent oxidation, lock the QDs into position, inhibit diffusion, and tune the height and width of the inter-QD potential barriers that govern charge transport [5,6]. Poor stability is a common feature of nanoscale electronic materials, yet stability is all too rarely the focus of basic research. Fundamental studies are therefore needed to elucidate the most important mechanisms of degradation and develop simple yet effective countermeasures. By revealing both how QD solids degrade in response to environmental stresses (oxidative, photothermal, and electric) and how to prevent this degradation, the project has greatly improved our ability to develop stable, high-performance QD materials for real-world applications.

36 MATERIALS SCIENCE↗

DOE OSTI2016

Supramolecular networks with electron transfer in two dimensions

Organic charge-transfer (CT) co-crystals in a crossed stack system are disclosed. The co-crystals exhibit bidirectional charge transfer interactions where one donor molecule shares electrons with two different acceptors, one acceptor face-to-face and the other edge-to-face. The assembly and charge transfer interaction results in a pleochroic material whereby the optical absorption continuously changes depending on the polarization angle of incident light.

36 MATERIALS SCIENCE↗

DOE OSTI2018

Supramolecular networks with electron transfer in two dimensions

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2019

Tin Nitride Atomic Layer Deposition Using N2H4

There is substantial lag in the development of atomic layer deposition (ALD) processes for nitrides compared to the high-quality, conformal oxides for which ALD has become the standard. A major factor in this disparity is the ready availability of highly reactive oxygen sources (mainly H2O, O2, and H2O2). High-energy nitrogen precursors are similarly required for the efficient incorporation of nitrogen in a film. Ammonia has often been used in conjunction with metal chlorides but requires relatively high temperatures for thermal ALD. Plasma-enhanced ALD can utilize molecular nitrogen as a precursor but can reduce film conformality on complex supports and damage the underlying substrate. Hydrazine (N2H4) is an alternative precursor which has been rarely explored for the fabrication of nitrides in ALD, but which is experiencing a surge in popularity due to its high reactivity, which enables the deposition of nitrides as-yet undemonstrated by ALD.(1) The added reactivity and volatility of liquid hydrazine may enable new reaction mechanisms, lower deposition temperatures, and conformality for high aspect ratio applications. Sn3N4 is a metastable semiconductor which shares a crystal structure with its analog, Si3N4; unlike Si3N4, Sn3N4 has only recently been grown by ALD,(2) being synthesized much more often through reactive sputtering.(3) As a binary, Sn3N4 has applications as a battery anode material, for photoelectrochemistry, and optoelectronic devices. We will report progress on the deposition of SnxNy films from tetrakis(dimethylamido) tin (TDMASn) and N2H4. Growth per cycle of this material (determined by x-ray reflectivity) is 0.4 A at 200 C, similar to the sole report of Sn3N4 from PE-ALD,(2) despite films being substantially Sn-rich. Identification of ALD growth window and self-limiting deposition characteristics are underway; initial testing indicates a competing chemical vapor deposition process which can be eliminated with adequate tuning of pulse/purge characteristics. A comparison of film conductivity and optical absorption at different growth temperatures will be presented. General issues of N2H4 purity and routes to prevent or control oxynitride formation will be discussed. (1) Du, L., et al. The First Atomic Layer Deposition Process for FexN Films. Chem. Comm., 2019, ASAP. DOI: 10.1039/C8CC10175B. (2) Stewart, D. M., et al. Tin Oxynitride Anodes by Atomic Layer Deposition for Solid-State Batteries. Chem. Mater. 2018, 30, 2526-34. (3) Caskey, C. M., et al. Semiconducting Properties of Spinel Tin Nitride and Other IV3N4 Polymorphs. J. Mater. Chem. C 2015, 3, 1389-96.

14 SOLAR ENERGY↗

DOE OSTI2020

Hydrophilic, light active coating for membranes

A porous membrane provides enhanced filtration of pollutants and particles by coating the membrane with conformal thin films of doped titanium dioxide via atomic layer deposition or, alternatively, sequential infiltration synthesis. The membrane can either be organic or inorganic, and the doping of the membrane, usually with nitrogen, is an important feature that shifts the optical absorption of the TiO2 from the UV range into the visible-light range. This enables the use of lower energy light, including sunlight, to activate the photocatalytic function of the film. The coating described in the present invention is compatible with virtually any porous membrane and allows for precise tuning of the pore size with molecular precision. The present invention presents a new coating process and chemical structure that provides catalytic activity, strongly enhanced by light, to both mitigate fouling and break down various organic pollutants in the process stream.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Metallo-graphene nanocomposites and methods for using metallo-graphene nanocomposites for electromagnetic energy conversion

Nanocomposites in accordance with many embodiments of the invention can be capable of converting electromagnetic radiation to an electric signal, such as signals in the form of current or voltage. In some embodiments, metallic nanostructures are integrated with graphene material to form a metallo-graphene nanocomposite. Graphene is a material that has been explored for broadband and ultrafast photodetection applications because of its distinct optical and electronic characteristics. However, the low optical absorption and the short carrier lifetime of graphene can limit its use in many applications. Nanocomposites in accordance with various embodiments of the invention integrates metallic nanostructures, such as (but not limited to) plasmonic nanoantennas and metallic nanoparticles, with a graphene-based material to form metallo-graphene nanostructures that can offer high responsivity, ultrafast temporal responses, and broadband operation in a variety of optoelectronic applications.

Jarrahi, Mona↗

DOE OSTI2023

Photoconductive metasurface-based ultrafast device

A theoretically perfectly absorbing photoconductive all-dielectric metasurface is provided. This metasurface can improve the efficiency and performance of ultrafast photoconductive switches and detectors. In an embodiment, the metasurface is incorporated in photoconductive THz switches or detectors. In embodiments, the metasurface is constituted by a network of gallium arsenide resonators. Each resonator supports two degenerate and critically coupled magnetic dipole modes. Simultaneous excitation of these two modes leads to theoretically close-to-perfect optical absorption near the resonant wavelength.

Brener, Igal↗

NASA NTRS2011

Two-Photon-Absorption Scheme for Optical Beam Tracking

A new optical beam tracking approach for free-space optical communication links using two-photon absorption (TPA) in a high-bandgap detector material was demonstrated. This tracking scheme is part of the canonical architecture described in the preceding article. TPA is used to track a long-wavelength transmit laser while direct absorption on the same sensor simultaneously tracks a shorter-wavelength beacon. The TPA responsivity was measured for silicon using a PIN photodiode at a laser beacon wavelength of 1,550 nm. As expected, the responsivity shows a linear dependence with incident power level. The responsivity slope is 4.5 x 10(exp -7) A/W2. Also, optical beam spots from the 1,550-nm laser beacon were characterized on commercial charge coupled device (CCD) and complementary metal-oxide semiconductor (CMOS) imagers with as little as 13.7 microWatts of optical power (see figure). This new tracker technology offers an innovative solution to reduce system complexity, improve transmit/receive isolation, improve optical efficiency, improve signal-to-noise ratio (SNR), and reduce cost for free-space optical communications transceivers.

Ortiz, Gerardo G.↗

NASA NTRS1992

Solar absorptance degradation of optical solar reflector radiators on the Spacenet satellites

Telemetry data are presented for two communications hybrid satellites, Spacenet I and Spacenet II, collected to determine the long-term temperature trend and associated solar absorptance degradation of the optical solar reflectors (OSRs). A thermal model was used to calculate the thermal sensitivity of various OSR components to changes in the solar absorptance and to determine absolute values of solar absorptance. The separation of the data into sunlit and nonsunlit periods made it possible to confirm the hypothesis that degradation occurs under the catalytic activity of direct sunlight on the spacecraft contaminants. The differences found between the degradation rates for Spacenet-I and Spacenet-II satellites and between the present results and published reports on other satellites are considered to be related to variations in the volume of spacecraft contaminants.

Naegeli, Charles R.↗

DOE OSTI2016

An organic dye-polymer (phenol red-poly (vinyl alcohol)) composite architecture towards tunable -optical and -saturable absorption characteristics

Herein, we demonstrate that blending an organic dye (guest/filler), with a vinyl polymer (host template), is an inexpensive and simple approach for the fabrication of multifunctional photonic materials which could display an enhancement in the desirable properties of the constituent materials and, at the same time provide novel synergistic properties for the guest-host system. A new guest-host nanocomposite system comprising Phenol Red dye and poly (vinyl alcohol) as guest and host template, respectively, which exhibits tunable optical characteristics and saturable absorption behavior, is introduced. The dependence of local electronic environment provided by the polymer template and the interactions of the polymer molecules with the encapsulated guest molecules on the observed optical/nonlinear absorption behavior is discussed. An understanding of the tunability of the optical/ photophysical processes, with respect to the filler content, as discussed herein could help in the design of improved optical materials for several photonic device applications like organic light emitting diodes and saturable absorbers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2016

Management of light absorption in extraordinary optical transmission based ultra-thin-film tandem solar cells

Although ultra-thin-film solar cells can be attractive in reducing the cost, they suffer from low absorption as the thickness of the active layer is usually much smaller than the wavelength of incident light. Different nano-photonic techniques, including plasmonic structures, are being explored to increase the light absorption in ultra-thin-film solar cells. More than one layer of active materials with different energy bandgaps can be used in tandem to increase the light absorption as well. However, due to different amount of light absorption in different active layers, photo-generated currents in different active layers will not be the same. The current mismatch between the tandem layers makes them ineffective in increasing the efficiency. In this work, we investigate the light absorption properties of tandem solar cells with two ultra-thin active layers working as two subcells and a metal layer with periodically perforated holes in-between the two subcells. While the metal layer helps to overcome the current mismatch, the periodic holes increase the absorption of incident light by helping extraordinary optical transmission of the incident light from the top to the bottom subcell, and by coupling the incident light to plasmonic and photonic modes within ultra-thin active layers. We extensively study the effects of the geometry of holes in the intermediate metal layer on the light absorption properties of tandem solar cells with ultra-thin active layers. We also study how different metals in the intermediate layer affect the light absorption; how the geometry of holes in the intermediate layer affects the absorption when the active layer materials are changed; and how the intermediate metal layer affects the collection of photo-generated electron-hole pairs at the terminals. We find that in a solar cell with 6,6-phenyl C61-butyric acid methyl ester top subcell and copper indium gallium selenide bottom subcell, if the periodic holes in the metal layer are square or polygon, total absorption remains approximately the same. However, the total absorption suffers significantly if the holes are triangle. The transmission spectra of incident light into the bottom subcell, and hence the absorption, change significantly for square and circle holes if the active materials change to cadmium selenide (CdSe) and cadmium telluride (CdTe) in the top and bottom subcells, respectively. Although the intermediate metal layer may induce electron-hole pair recombination due to surface defects, the short-circuit current density of an ultra-thin plasmonic solar cell with an intermediate metal layer with two-dimensional hole array is >9% of that of a structure without the intermediate metal layer.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1973

Spectral line absorption measurement using optical cavities.

A simple technique using a conventional gas laser with spherical mirrors having identical radii of curvature in the nonoscillating regime for spectral line absorption measurements is described and applications for laser work are suggested. The theory of the measurement carried out in the geometrical optical approach for Doppler-broadened lines was checked experimentally and conditions are specified for which measurement inaccuracies of the order of 1% for the peak value of the line absorption coefficient can be obtained. Since the device provides a fine adjustment of the cavity losses, formation of the diffraction modes could be observed in the preoscillating regime of the optical cavity.

Blanaru, D. L.↗

DOE OSTI2016

Study of atmospheric scattering and absorbing aerosols at 550 nm over nearby western Indian tropical sites of Thar Desert effected region

The first time experimental results based on spaced satellite observations of different kinds of aerosols properties have been described over two different contrast environmental conditions locations in western tropical Indian region specifically first at Jaisalmer (26.90°N, 69.90°E, 220 m above mean sea level (amsl)) located in central Thar dessert vicinity of western Indian site over Indian Thar Desert region and another at Udaipur (24.6° N, 73.7° E, 560 m amsl) site concerning to semi-urban and semi arid place of hilly areas. The daily values of aerosols optical depth absorption at 500nm (AOD abs 500nm), aerosols optical depth extinction at 500nm (AOD ext 500nm) along with aerosols optical depth at 500nmon (AOD 500nm) of eleven year period from Jan., 2004 to Dec., 2014 are basis of primary database of the present investigation. From the synthesis if the above database and the basis of rigorous statistical approach, following some of interesting facts are noted (i) larger annual monthly AOD variation of 0.93 is noted over JSM when compared to observed annual monthly change in AOD cycle, over UDP, of only 0.50 clearly indicating the more impact of desert influence activities about more than double times over JSM than UDP (ii) The higher abundance of absorbing aerosols occurrences about two time higher are seen in JSM in comparison to UDP. It indicates the clear evidence of strong optical absorption properties of useful solar mid visible wavelength at 550nm as the results of presence of more availability of dust aerosols as mineral natural type in pre-monsoon to post-monsoon over JSM which is also more predominant over JSM than the UDP region located far away from desert activity regime (iii) The greater sharing of extinction solar radiation effect on aerosols are more effective in pre-monsoon in UDP in reference to over JSM, where as in case of UDP, the aerosols effect through the scattering mechanism gradually reduce from monsoon to winter months as compared to observed over JSM. The more detailed analysis other important results are also discussed thoroughly in this paper.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2020

Dynamic computational optical fringe mitigation in tunable laser absorption spectroscopy

In optical spectroscopic systems where unwanted optical scattering cannot be eliminated, Fabry-Pérot etalons cause unpredictable changes in the spectral background. Frequent system calibration is then required to maintain the desired measurement accuracy, which presents a major limitation to the spectrometer. We introduce a computational approach to mitigate the adverse effects of optical fringing without hardware modifications. Motivated by experimental observations of complicated fringe behaviors, we simplify the problem by decomposing the fringe background into component etalons that can be addressed according to their individual characteristics. The effectiveness of the proposed method is demonstrated on a silicon photonic methane sensor, where accurate measurements of methane concentration are obtained from spectral data strongly affected by optical fringes.

Teng, Chu C. (ORCID:0000000152744835)↗

NASA NTRS2000

Optical Control of Intersubband Absorption in a Multiple Quantum Well-Embedded Semiconductor Microcravity

Optical intersubband response of a multiple quantum well (MQW)-embedded microcavity driven by a coherent pump field is studied theoretically. The n-type doped MQW structure with three subbands in the conduction band is sandwiched between a semi-infinite medium and a distributed Bragg reflector (DBR). A strong pump field couples the two upper subbands and a weak field probes the two lower subbands. To describe the optical response of the MQW-embedded microcavity, we adopt a semi-classical nonlocal response theory. Taking into account the pump-probe interaction, we derive the probe-induced current density associated with intersubband transitions from the single-particle density-matrix formalism. By incorporating the current density into the Maxwell equation, we solve the probe local field exactly by means of Green's function technique and the transfer-matrix method. We obtain an exact expression for the probe absorption coefficient of the microcavity. For a GaAs/Al(sub x)Ga(sub 1-x)As MQW structure sandwiched between a GaAs/AlAs DBR and vacuum, we performed numerical calculations of the probe absorption spectra for different parameters such as pump intensity, pump detuning, and cavity length. We find that the probe spectrum is strongly dependent on these parameters. In particular, we find that the combination of the cavity effect and the Autler-Townes effect results in a triplet in the optical spectrum of the MQW system. The optical absorption peak value and its location can be feasibly controlled by varying the pump intensity and detuning.

Liu, Ansheng↗

NASA NTRS1996

Absorption Filter Based Optical Diagnostics in High Speed Flows

Two major regimes where laser light scattered by molecules or particles in a flow contains significant information about the flow are Mie scattering and Rayleigh scattering. Mie scattering is used to obtain only velocity information, while Rayleigh scattering can be used to measure both the velocity and the thermodynamic properties of the flow. Now, recently introduced (1990, 1991) absorption filter based diagnostic techniques have started a new era in flow visualization, simultaneous velocity and thermodynamic measurements, and planar velocity measurements. Using a filtered planar velocimetry (FPV) technique, we have modified the optically thick iodine filter profile of Miles, et al., and used it in the pressure-broaden regime which accommodates measurements in a wide range of velocity applications. Measuring velocity and thermodynamic properties simultaneously, using absorption filtered based Rayleigh scattering, involves not only the measurement of the Doppler shift, but also the spectral profile of the Rayleigh scattering signal. Using multiple observation angles, simultaneous measurement of one component velocity and thermodynamic properties in a supersonic jet were measured. Presently, the technique is being extended for simultaneous measurements of all three components of velocity and thermodynamic properties.

Samimy, Mo↗